![Development of chitosan-nano-silicon aerogel films incorporated with Okara powder by casting method. Reprinted/adapted with permission from Ref. [156]. 2020, Elsevier.](https://www.researchgate.net/publication/371767235/figure/fig2/AS:11431281169649962@1687437050674/Development-of-chitosan-nano-silicon-aerogel-films-incorporated-with-Okara-powder-by_Q320.jpg)
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Citation: Perera, K.Y.; Jaiswal, A.K.;
Jaiswal, S. Biopolymer-Based
Sustainable Food Packaging
Materials: Challenges, Solutions, and
Applications. Foods 2023,12, 2422.
https://doi.org/10.3390/
foods12122422
Academic Editors: Hanna
(John) Khouryieh and Jianhua Xie
Received: 6 May 2023
Revised: 6 June 2023
Accepted: 7 June 2023
Published: 20 June 2023
Copyright: © 2023 by the authors.
Licensee MDPI, Basel, Switzerland.
This article is an open access article
distributed under the terms and
conditions of the Creative Commons
Attribution (CC BY) license (https://
creativecommons.org/licenses/by/
4.0/).
foods
Review
Biopolymer-Based Sustainable Food Packaging Materials:
Challenges, Solutions, and Applications
Kalpani Y. Perera 1,2 , Amit K. Jaiswal 1,2,* and Swarna Jaiswal 1,2
1Sustainable Packaging and Bioproducts Research (SPBR) Group, School of Food Science and Environmental
Health, Faculty of Sciences and Health, Technological University Dublin, City Campus, Grangegorman,
D07 ADY7 Dublin, Ireland; kalpani.gamage@tudublin.ie (K.Y.P.); swarna.jaiswal@tudublin.ie (S.J.)
2Environmental Sustainability and Health Institute, Technological University Dublin, City Campus,
Grangegorman, D07 H6K8 Dublin, Ireland
*Correspondence: amit.jaiswal@tudublin.ie; Tel.: +353-1-220-5661
Abstract:
Biopolymer-based packaging materials have become of greater interest to the world due to
their biodegradability, renewability, and biocompatibility. In recent years, numerous biopolymers—
such as starch, chitosan, carrageenan, polylactic acid, etc.—have been investigated for their potential
application in food packaging. Reinforcement agents such as nanofillers and active agents improve the
properties of the biopolymers, making them suitable for active and intelligent packaging. Some of the
packaging materials, e.g., cellulose, starch, polylactic acid, and polybutylene adipate terephthalate,
are currently used in the packaging industry. The trend of using biopolymers in the packaging
industry has increased immensely; therefore, many legislations have been approved by various
organizations. This review article describes various challenges and possible solutions associated
with food packaging materials. It covers a wide range of biopolymers used in food packaging
and the limitations of using them in their pure form. Finally, a SWOT analysis is presented for
biopolymers, and the future trends are discussed. Biopolymers are eco-friendly, biodegradable,
nontoxic, renewable, and biocompatible alternatives to synthetic packaging materials. Research
shows that biopolymer-based packaging materials are of great essence in combined form, and further
studies are needed for them to be used as an alternative packaging material.
Keywords:
biopolymers; food packaging materials; bioplastics; sustainability; biopolymer-based
materials; SWOT analysis
1. Introduction
The use of biopolymers as packaging materials is becoming an emerging trend world-
wide due to their major benefits over plastics, such as biodegradability, eco-friendly nature,
nontoxicity, and biocompatibility. These natural biopolymers have excellent film-forming
cohesive structures and thin protective layers of film [1].
Biopolymers used as food packaging materials are mainly polysaccharides, proteins,
and aliphatic polyesters, which can maintain food quality and increase the shelf-life of the
product. These packaging materials [
1
] have barrier properties that control the exchange
of gases, moisture, aroma, and lipids from the external environment and vice versa, [
2
]
possess antimicrobial activity that can protect the food product from the external environ-
ment, and [
3
] prevent the loss of desirable compounds such as flavor and texture [
2
–
4
].
Biopolymers such as starch, cellulose, and polylactic acid (PLA) are currently used for food
packaging materials. However, the main limitation of using biopolymers in food packaging
is their weak mechanical strength and high sensitivity to moisture. The merits and demerits
differ depending on the type of biopolymer used for food packaging. Table 1shows the
advantages and disadvantages of different biopolymers used in food packaging. To over-
come the weaknesses of biopolymers, many studies have been performed with the addition
of reinforcing agents such as nanofillers, biopolymers, plasticizers, and natural agents
Foods 2023,12, 2422. https://doi.org/10.3390/foods12122422 https://www.mdpi.com/journal/foods
Foods 2023,12, 2422 2 of 59
such as essential oils. Furthermore, biopolymer matrices act as carriers for antimicrobial
substances, antioxidants, flavor agents, vitamins, or nutrients, thereby aiding in improving
food quality, safety, nutritional value, and sensory properties. An overview of biopolymers
in food packaging is presented in Figure 1. Due to the numerous advantages, biopolymers
have been proposed as an alternative to synthetic polymers such as plastic, which reduces
the harmful impact on the environment [
5
]. As the use of biopolymers in food packaging
materials is increasing, it is important to upgrade the biopolymer industry to a large scale.
Strategies for sourcing biopolymers include utilizing agricultural waste, instituting efficient
cultivation practices, and researching innovative biopolymer production technologies.
Table 1. Advantages and disadvantages of different biopolymers in food packaging.
Biopolymer Positive Characteristics Negative Characteristics References
Starch-based biopolymers
Starch
•Biodegradable
•Renewable
•Nontoxic
•Low cost
•Abundance
•Transparent
•colorless, flavorless, tasteless
•Good lipids, oxygen, UV barrier properties
•Great film-forming ability
•Low water vapor permeability
•Limited process ability
•Poor water resistance
•Low mechanical properties
•Hydrophilic
•Low thermal properties
•Brittleness
[1,6–9]
Chitosan
•Biodegradable
•Renewable
•Nontoxic
•Increased absorption properties
•High antimicrobial activity
•High biocompatibility
•Low production cost
•
Good gas, aroma, UV, oil barrier properties
•Wettability
•Antioxidant properties
•water-insoluble
•Good film-forming ability
•Good optical properties
•Transparent
•Flexible
•Low mechanical properties
•High hydrophobicity
•Low water vapor barrier
properties
•Brittleness
•Low elasticity
[10–12]
Carrageenan
•Biodegradable
•Renewable
•Nontoxic
•Good gas, moisture barrier properties
•Thermal stability
•Antibacterial properties
•Excellent film-forming ability
•Transparent
•Poor mechanical properties
•Low water vapor barrier
properties
•Water resistance properties
[13–17]
Foods 2023,12, 2422 3 of 59
Table 1. Cont.
Biopolymer Positive Characteristics Negative Characteristics References
Cellulose
•Biodegradable
•Renewable
•Nontoxic
•Low energy consumption
•High surface area
•Good oxygen, hydrocarbon barrier
properties
•High mechanical strength
•High water vapor permeability
•Low cost
•Low density
•High specificity
•Biocompatibility
•Odorless, tasteless
•Chemical stability
•Low mechanical strength
•Opacity
•Enhanced color value
•Hydrophilic nature
•Poor water vapor barrier
properties
[18–21]
Agar
•Biodegradable
•Renewable
•Nontoxic
•Good film-forming ability
•Stability in different environment
conditions
•Transparent
•Poor water vapor barrier
properties
•Poor mechanical properties
•Brittleness
•Poor thermal stability
•Strong hydrophilic characteristic
[3,4,22–24]
Pectins
•Biodegradable
•Renewable
•Nontoxic
•Good oil, aroma, gas barrier properties
•High mechanical properties
•Good rheological properties
•Cost effective
•Good film-forming capacity
•Ineffective against moisture
transfer
•Poor mechanical properties
•Brittleness
•Poor thermal stability
•High water solubility
•Lack of antimicrobial properties
[25–28]
Alginate
•Biodegradable
•Renewable
•Nontoxic
•Control swelling properties
•Low cost
•Biocompatibility
•Good mechanical properties
•Chemical stability
•Good water barrier properties
•Good mechanical properties
•Stiffness
•Maintaining the flavor
•Retarding fat oxidation
•Brittleness
•Poor moisture barriers
•Poor water resistance
•High water vapor permeability
•High hydrophilicity
[29–33]
Gums
•Biodegradable
•Renewable
•Nontoxic
•Control viscosity
•Biocompatibility
•Low cytotoxicity
•High cost of production
•Low rheological properties
•Low mechanical properties
•Low barrier properties
[34–36]
Foods 2023,12, 2422 4 of 59
Table 1. Cont.
Biopolymer Positive Characteristics Negative Characteristics References
Lignin
•Biodegradable
•Renewable
•Nontoxic
•Natural broad UV blocker
•Antioxidant properties
•Low mechanical properties
•Low barrier properties [4,34,37,38]
Pullulan
•Biodegradable
•Renewable
•Nontoxic
•Odorless, tasteless, colorless
•Flexible
•Transparent
•Thermal stability
•Good oil, oxygen barrier properties
•Biocompatibility
•Heat-sealable
•water permeable
•Low mechanical properties
•Brittleness
•Low water resistance
•Moisture sensitivity
[20,39,40]
Curdlan
•Biodegradable
•Renewable
•Nontoxic
•Colorless, odorless
•High absorption
•Water insoluble
•Thermal stability
•Poor mechanical properties [41,42]
Protein-based biopolymers
Gelatin
•Biodegradable
•Renewable
•Nontoxic
•Low cost
•Abundant
•Excellent film-forming ability
•Biocompatible
•Flexible
•Transparent
•Excellent water, UV, aroma oxygen barrier
properties
•Low water vapor permeability
•Poor swelling properties
•Low tensile strength
•Opacity
•High roughness
•Poor mechanical properties
•Poor processability
[24,43–45]
Soy protein
•Biodegradable
•Renewable
•Nontoxic
•Good oxygen, lipid barrier properties
•Abundance
•Low cost
•Biocompatibility
•Excellent film-forming capacity
•High water vapor permeability
•Low water resistance
•Low thermoplasticity
•Brittleness
•Low mechanical properties
•Low film gloss
•Low tensile strength
•Poor plasticity
•Low water vapor permeability
[46–49]
Foods 2023,12, 2422 5 of 59
Table 1. Cont.
Biopolymer Positive Characteristics Negative Characteristics References
whey proteins
•Biodegradable
•Renewable
•Nontoxic
•Tasteless, flavorless
•Flexible
•Transparent
•Soft
•Elastic
•water-insoluble
•Good gas, aromatic, grease barrier, oxygen
barrier properties
•Low cost
•Nutritional value
•Excellent film-forming ability
•Weak resistance to moisture
•Low mechanical properties [50–53]
zein
•Biodegradable
•Renewable
•Nontoxic
•Good oxygen/gas barrier properties
•High thermal resistance
•High tensile strength
•Hydrophobic properties
•High antimicrobial potential
•Good antioxidant properties
•Form adhesive film
•High toughness
•Low water vapor permeability
•Low flexibility
•Low mechanical strength
•Brittleness
•High relative humidity condition
•Poor processability
•Low elongation at break
•Weak thermal properties
•Weak mechanical properties
•Rapid dissolution rate
•Low gas permeability
[54–57]
Keratin
•Biodegradable
•Renewable
•Nontoxic
•Hydrophobic properties
•Poor mechanical properties [58,59]
Collagen
•Biodegradable
•Renewable
•Nontoxic
•Excellent film formation ability
•Biocompatibility
•Antioxidant properties
•Good moisture, oxygen barrier properties
•Ensure structural integrity
•Poor mechanical strength
•High water vapor permeability [60]
Aliphatic polyester-based biopolymers
Poly lactic acid
(PLA)
•Biodegradable
•Renewable
•Nontoxic
•Good flavor, odor
•Antimicrobial properties
•Transparent
•Good oil, oxygen barrier properties
•Good mechanical strength
•Light transmission
•Rigidity
•Low cost
•High stiffness
•Flexibility
•Biocompatibility
•Brittleness
•Low mechanical properties
•Low thermal stability
•Low melt strength
[61–65]
Foods 2023,12, 2422 6 of 59
Table 1. Cont.
Biopolymer Positive Characteristics Negative Characteristics References
poly(butylene
adipate
terephthalate)
(PBAT)
•Biodegradable
•Renewable
•Nontoxic
•Flexible
•Good oxygen barrier
•Chemical inactivity
•High viscosity
•Good mechanical properties
•Low water vapor permeability
•Poor resistance
•Poor impact resistance
•High cost of production
•Low thermal properties
•Low antimicrobial activity
•Poor photostability
•Low mechanical performance
•Low crystallization rate
[9,63,66]
Poly caprolactone
(PCL)
•Biodegradable
•Renewable
•Nontoxic
•Excellent ability to form blends
•Poor mechanical properties
•Poor thermal properties
•High solubility [57]
polybutylene
succinate (PBS)
•Biodegradable
•Renewable
•Nontoxic
•High crystallinity
•Good thermal properties
•Good mechanical properties
•Poor barrier properties [67]
Polyhydroxyalkanoate
(PHAs)
•Biodegradable
•Renewable
•Nontoxic
•Good tensile strength
•Flavor, odor
•Good oxygen, water barrier properties
•Temperature stability
•Biocompatible
•High cost
•Low thermal properties
•Low mechanical properties [68–70]
Despite numerous works reporting on the use of biomaterials for packaging [
61
,
71
,
72
],
the novelty of this review lies in the extensive explanation of each material’s unique
qualities that make it appealing for packaging a specific food product. This review article
also describes various challenges and possible solutions associated with food packaging
materials. It examines the current state of research and industrial application, including
the advantages and disadvantages of various biopolymer-based food packaging. Finally,
a SWOT (strengths, weaknesses, opportunities, and threats) analysis is performed on
biopolymers, and future trends are discussed. Thus, this review will be useful in the
decision-making process to develop biopolymer-based packaging materials.
Foods 2023,12, 2422 7 of 59
1
Figure 1. An overview of biopolymers in food packaging (Figure created with BioRender).
2. Current Food Packaging Materials and Associated Issues/Challenges
Plastic, a petroleum-based, diverse, and ubiquitous material, is widely used in food
packaging due to its lightweight, cost-effective, transparent, versatile, and easy-to-process
properties [
1
,
5
]. These synthetic polymers possess excellent mechanical, thermal, and
barrier characteristics [
1
,
5
], while ultra-thin layers extend the shelf-life of packaged products
and reduce food waste [
5
]. Consequently, plastics provide direct economic benefits by
lowering transportation costs.
Global plastic production has increased significantly, with 40% of all produced plastic
being used for packaging, and nearly half of that for food packaging [
47
,
73
,
74
]. Europe’s
plastic distribution demand is dominated by packaging at 39.6% [
75
]. However, plastic’s
high production volume, short usage time, non-biodegradable nature, and inadequate
management have raised concerns worldwide, with recycling challenges arising from
multilayer plastics [5,47,76].
Plastics account for about 6% of global oil consumption, projected to increase to 20%
by 2050 [
5
]. Plastic waste damages terrestrial environments and pollutes aquatic ones,
accumulating due to prolonged degradation. Landfill plastics release harmful substances
during abiotic and biotic degradation, contaminating soil and water [
77
]. Chlorinated
plastics leach toxic chemicals, polluting ecosystems, while plastic degradation in water
releases chemicals such as polystyrene and Bisphenol A, causing water pollution [
77
].
Methane and CO
2
emissions during plastic microbial digestion contribute to global warm-
ing [
77
]. Animals are exposed to plastic waste through ingestion and entanglement, with
detrimental consequences.
Countries are addressing plastic pollution through waste reduction, production re-
duction, recycling, and alternatives [
77
]. Governments have adopted policy initiatives
to reduce plastic pollution, with global legislation focusing on protecting territorial and
marine environments. The United Nations Convention on the Law of the Sea (UNCLOS)
in 1982 was the first international legislation agreement on plastic waste [
77
]. Other con-
ventions include the International Convention for the Prevention of Pollution from Ships
(MARPOL) in 1973, the London Convention (1972), the Global Program Action for the
Protection of the marine environment from land-based activities (GPA) in 1995, and the
Global Partnership on Marine Litter (GPML) formed in 2012 [77].
The 17 Sustainable Development Goals (SDGs) by the United Nations General Assem-
bly in 2015 aim to promote sustainability, protect ecological life support systems, and reduce
Foods 2023,12, 2422 8 of 59
waste and pollution by 2030 [
77
]. The Basel Convention (1989), Rotterdam Convention
(2004), and Stockholm Convention (2004) address the safe disposal and management of
hazardous substances associated with plastic disposal [
77
]. Legislation on global warming
includes the United Nations Framework Convention on Climate Change (1992) (UNFCCC)
and the Montreal Protocol (1987) [77].
The European Union (EU) combats plastic pollution through strategic legislation,
including the EU action plan in 2015, the Regional Strategy for Plastics in a Circular
Economy in 2018, and the directive on the reduction in the impact of certain plastic products
in 2019 [
78
,
79
]. The latest update in 2020 focuses on the regulation of recycled content,
waste reduction, and product labeling [75].
3. Possible Solutions for Current Food Packaging Materials
The growing environmental concerns surrounding plastics have prompted research
into alternative food packaging materials [
79
]. Biodegradable materials, such as biopolymers,
bioplastics, bio-nanocomposites, and edible coatings, are being developed to replace plastics.
Biodegradable polymers are renewable, nontoxic, biodegradable, biocompatible, repro-
ducible, versatile, abundantly available, and boast a low carbon footprint [
3
,
47
]. However,
issues such as viscosity, hydrophobicity, crystallization activity, brittleness, water sensitivity,
thermal stability, gas barrier properties, mechanical strength, processing difficulty, and
cost have hindered their widespread industrial adoption [
2
]. Biodegradable polymers
can be classified as polysaccharides (starch, cellulose, chitosan, etc.), proteins (soy protein,
collagen, zein, etc.), and aliphatic polyesters (polybutylene adipate terephthalate (PBAT),
PLA, etc.) [1].
To address these issues, biodegradable polymers can be blended with other biodegrad-
able polymers, plasticizers (e.g., glycerol), and compatibilizers (e.g., essential oils) [
2
,
3
,
80
].
The biopolymer packaging market in Europe increased from 1743.9 million m
2
in 2016 to
2427.1 million m
2
in 2021 [
78
]. Bioplastics are bio-based and/or biodegradable plastics that
share properties with traditional plastics and offer additional benefits such as renewability
and biodegradability [81].
Bio-nanocomposites, which consist of a bio-based polymer matrix and an organic/inorganic
filler with at least one nanoscale material, are suitable as active and/or intelligent packaging
materials due to their enhanced mechanical, thermal, barrier, antimicrobial, and antioxidant
properties [
82
–
84
]. These materials focus on extending shelf-life and reducing microbial
growth in food products [83,84].
Biopolymer-based edible films, formed from polysaccharides or blends of polysac-
charides containing proteins, lipids, and food-grade additives, are suitable for human
consumption and can increase the shelf-life and quality of food products [
85
,
86
]. Despite
their potential, these packaging techniques confront obstacles such as poor elongation,
safety and health concerns, high cost, processing difficulties, lack of awareness, cultural
concerns, and customer acceptance [87].
4. Degradation Chemistry of Biopolymers
During biopolymer biodegradation, the polymers are first converted to monomers,
and they are then mineralized. The mineralization of the organic material takes place by
microorganisms (e.g., fungi, archaea, and bacteria) eventually resulting in carbon diox-
ide, water, and biomass. The reactions occurring during biopolymer biodegradation
are as below:
Biodegradable polymers →CO2+ H2O + biomass
The biodegradation of the large molecules of the biopolymers takes place by extracel-
lular enzymes in microorganisms, while the smaller molecules are transported into the mi-
croorganism digestion by endoenzymes. For the biodegradation of a biopolymer substrate,
most microorganisms use multiple enzyme systems. The biopolymer biodegradation takes
place either through oxo-biodegradation or hydro-biodegradation. Oxo-biodegradation
takes place in natural polymers such as rubber, humus, and lignin. During this process,
Foods 2023,12, 2422 9 of 59
loss of the mechanical properties of carbohydrate polymers takes place by the peroxidation
process, which is initiated by heat/light, resulting in oxocarboxylic acid molecules, alde-
hydes, ketones, and alcohols. After that, the biopolymers undergo bio-assimilation with
the aid of enzymes of microorganisms into the water, carbon dioxide, and biomass. The
hydro-biodegradation process takes place in cellulose, starch, and aliphatic polyesters. The
biopolymers are converted into monomers through the enzymatic digesting of microorgan-
isms. The hydrolysis of ester bonds in monomers is performed by the extracellular enzymes
of microorganisms. The aliphatic polyesters and carbohydrate polymers are hydrolyzed
and bio-assimilated rapidly in an aqueous medium [88].
The rate of biodegradation depends upon different factors such as (1) polymer char-
acteristics (chemical bonds, branching, hydrophilicity/hydrophobicity, stereochemistry,
molecular weight, chain flexibility, crystallinity, interactions with polymers, coatings, sur-
face area, mobility, and addition of plasticizers/additives/active agents), (2) microorganism
type (aerobic and anaerobic facultative, co-metabolism, nature, enzymes, enzyme level,
enzyme location, enzyme kinematics, and inhibitors/ inducers), and (3) environment con-
ditions (temperature, humidity, oxygen, salts, metals, trace nutrients, pH, redox potential,
stability, pressure, alternate carbon, and light). When the above conditions are present
appropriately, the rapid degradation process occurs. During industrial composting, the
bioplastics are biodegraded in approximately 6–12 weeks [89].
To access the biodegradability of a biopolymer, laboratory tests, simulation tests, and
field tests are carried out. The laboratory tests applied include enzyme tests, clear zone
tests, Sturm tests, and synthetic environment-defined conditions. Stimulation tests are
performed using laboratory reactors, water, soil, compost, and material from landfills with
complex environments in defining conditions. Finally, field tests are performed in nature,
water, and soil/compland fill under a complex environment in variable conditions [90].
5. Important Properties of Biopolymers in Food Packaging
The properties of the packaging materials, such as barrier, mechanical, chemical, and
thermal properties, play an important role in increasing the shelf-life and maintaining the
quality of the food products. The barrier properties of a biopolymer used in food packaging
are the main parameter for extending the shelf-life of the packed food product. Barrier
properties such as gas, water vapor, organic vapors, and liquids are essential for food
packaging to separate the food product from the external environment. In addition, these
products differ in the different biopolymers used in food packaging. Thus, the loss/gain
of oxygen and water plays a major role in food deterioration. The barrier properties
play a crucial role in packaging since gas/water vapor may pass through the walls of the
biopolymer, resulting in changing the food product quality and shelf-life [91,92].
The gas permeability of the packaging material depends on the parameters; trans-
mission rate, permeance, and permeability. However, the barrier properties of materials
not only depend on these factors but also on environmental conditions such as temper-
ature, pressure, and relative humidity. Further, the rating of the barrier properties also
depends on the nature of the food products that are to be packaged. As a result, food
packaging materials can prolong the shelf-life of food products by improving the barrier
properties [93].
The oxygen barrier properties of a packaging material play an important role in the
preservation of fresh food products. The oxygen permeability is quantified by the oxygen
transmission rate and oxygen permeability [
93
]. This measures the amount of oxygen in
the packaging system. When the oxygen permeability is reduced, the oxygen pressure in
the packaging system drops, resulting in an extended shelf-life of the food product [93].
The water vapor barrier properties are of great significance for food products to
maintain physical or chemical deterioration concerning the moisture content. The water
vapor barrier properties are quantified by the water vapor permeability of the packaging
material by the ASTM E-96-95 standard method and the water vapor transmission rate [
94
].
The water vapor permeability depends upon the solubility and the diffusion of the water in
Foods 2023,12, 2422 10 of 59
the polymer material. The shelf-life of some food products is directly related to the water
exchange rate between the external and internal environment; thus, the water transfer
should be reduced to protect the food product from moisture [95].
The UV barrier properties of packaging material are quantified by the optical prop-
erties of a film using a spectrophotometer [
96
]. The UV barrier properties are essential to
prevent the loss of nutrient value and the change in the color of food [29].
Mechanical properties of the packaging system are essential to secure the food during
stressful conditions such as storage, handling, and processing of the food. The architecture
of the polymer matrix is the key factor that determines the mechanical properties of the
biopolymer. The mechanical properties of packaging material are determined by tensile
properties such as tensile strength, elongation at break, and elastic modulus [30,34,97].
Chemical resistance is important because the food in the package may be acidic and
combine with the packaging material. For safety reasons, it is important to find out what
the food is made of chemically before packing it. When these chemicals combine with and
become absorbed by the biopolymer matrix, the mechanical properties of the material may
change [92].
The thermal properties of the packaging material are determined by thermogravimetric
and differential scanning calorimetry. Thermal properties and thermal stability are essential
for the heat resistance of the packaging material. Thus, the thermal properties allow
us to store and transport the food packaging at the temperature essential for the food
products [57].
6. Biodegradable Polymers Currently Used in the Food Packaging Industry
6.1. Polysaccharide-Based Biopolymers
Polysaccharide-based biopolymers are nontoxic, abundantly available natural compo-
nents that are highly suitable as food packaging materials. They have excellent mechanical
and structural properties while being selectively permeable to carbon dioxide and oxygen.
However, they have poor water vapor barrier properties [66,97,98].
The biodegradable films from biodegradable polymers have been modified by the
addition of various reinforcement agents to produce a packaging system that has beneficial
properties and is suitable for industrial applications. Such films may include polymer
blending/hybrid films, plasticizers, and/or nanoparticles (NPs). The addition of antioxi-
dants, antimicrobials, nutrients, and color change indicators such as essential oils, phenolic
compounds, and plant extracts to biopolymers make them attractive, active, and intelligent
packaging, increasing the shelf-life of food. The addition of plasticizers (such as glyc-
erol/sorbitol) to biopolymers can modify their brittleness, increase their processing ability,
increase the mobility of starch chains, and decrease moisture absorption. Unfortunately,
the incorporation of plasticizers into biodegradable polymers decreases their mechanical
properties [6,23].
To improve the properties of the polysaccharides and develop them into an industrially
used active/smart packaging system, a combination of polysaccharides, lipids, and NPs
are utilized as explained in detail below in the different sub-sections of polysaccharides
(Table 2). The mechanical properties of some of the studies depicted in Table 2have been
taken, and a scatter plot has been drawn for a better understanding of the properties,
which can be seen in Figure 2. The active polysaccharides can be extracted using different
methods, such as hot water extraction, acid–base extraction, enzyme extraction, ultrasonic
extraction, ultrahigh pressure extraction, microwave extraction, and supercritical fluid
extraction [
97
]. Currently, starch blends and cellulose are used in industrial applications.
Products such as cups, plates, cutlery, and food packs are produced from thermoplastic
starch. Companies such as Plantic Technologies (Plantic, USA), Rodenburg Biopolymers
(Solanyl, Tokyo, Japan), Biotec (Bioplast, Bristol, PA, USA), Biop (Biopar, Schwalbach am
Taunus, Germany), Novamont (Mater Bi, Bottrighe, Italy/Waltham, MA, USA), KINGFA
(ECOPOND
®
, Guangzhou, China), and Biome Bioplastics Limited (BIOME Bioplastics,
Southampton, UK) manufacture starch-based films [
81
,
99
]. Additionally, cellulose is used in
Foods 2023,12, 2422 11 of 59
industries to make bags, wraps for food, and films. Companies such as Nature Works LLC
(BioMass Packaging
®
, Richmond, CA, USA) and Nature Flex
™
(Innovia Films, Wigton, UK)
produce these cellulose biopolymers on a large scale. Nature Flex
™
manufactures cellulose-
based products such as coffee and tea packaging, compostable snack bags, packaging for
dried foods, compostable stick packs, packaging for chocolate and candy, compostable
packaging, packaging for bakeries, custom packaging for food service, and compostable
bags. In addition, cellulose and chitosan-lined paper bags and cups are also produced at
the industrial level.
1
Figure 2.
Elongation at break versus tensile strength for polysaccharide-based biopolymers. Abbrevi-
ations: CNF-cellulose nanofibers, GG—Gellan gum, MMT—montmorillonite, SA—sodium alginate,
CMC—carboxymethyl cellulose, Pec—pectin, Pul—pullulan, Car—carrageenan, SP—soy protein,
Cur—Curdlan, Xan—xanthan.
6.1.1. Starch
Starch is a polysaccharide composed of linear (amylose) and branched (amylopectin)
sections, which are extracted from maize, potato, cassava, and cereal grains. It is regarded
as one of the most promising biodegradable polymers for use in food packaging due to
its many advantageous properties, such as biodegradability, low cost, abundance, trans-
parency, colorlessness, flavorlessness, tastelessness, reduced water sensitivity, excellent
oxygen barrier properties, renewability, edibility, and being an excellent film-forming
biopolymer. Nevertheless, starch alone is not a suitable food packaging material as it
lacks basic important properties such as vapor barrier, mechanical, and thermal properties.
It is also found to be brittle due to the massive inter- and intra-molecular interactions
between starch chains and is hydrophilic [
4
,
6
,
7
,
30
,
100
–
103
]. The two main techniques, the
dry process, and the wet process, are used for the development of starch biofilms [104].
Some limitations of using starch as a packaging material can be overcome by chemical
or physical modification of native starch. Chemical modification has limitations since
it is a complex, time-consuming process that can be toxic. The physical modification of
starch such as microwave treatment, pulsed electric field processing, and high-pressure
and irradiation treatments has yielded promising results [
105
]. Thermoplastic starch (TPS)
is developed by transforming the starch into a melted material by adding a plasticizer.
However, TPS also has poor mechanical and water vapor barrier properties, which make it
unsuitable for food packaging without the addition of other components [
8
,
106
]. Another
Foods 2023,12, 2422 12 of 59
modification of starch is the development of starch-based aerogels, which have been highly
studied and are still in the basic research stage. These aerogels are environmentally friendly,
biodegradable, and have many unique properties. The two main fabrication routes of
starch-based aerogels based on their shapes are monolith and microsphere [
101
]. Moreover,
starch nanocrystals are produced from native starch, which has many merits, such as high
surface area, robust mechanical properties, and intriguing self-assembly properties [
107
].
Starch foam packaging is an alternative packaging that was developed for polystyrene
foam in the initial research phase [103].
The incorporation of starch with other biodegradable polymers or synthetic poly-
mers allows for better packaging material. Recent studies by Lan et al. [
108
] focused on
encapsulating Lactococcus lactis into a starch-carboxymethyl cellulose matrix to form an
antimicrobial edible film as shown in Figure 3with low moisture content. The film con-
taining 1.5% L. lactis had the lowest water vapor transmission rate (5.54 g/m s Pa) and
retained a viable count of 5.64 log CFU/g of L. lactis after 30 days. After 8 days, the film
containing 1.5% L. lactis had the maximum nisin release (3.35 mg/mL) and antibacterial
efficacy against Staphylococcus aureus (53.53%).
2
Figure 3.
Antimicrobial edible film encapsulating Lactococcus lactis into a starch-carboxymethyl
cellulose matrix. Reprinted/adapted with permission from Ref. [108]. 2021, Elsevier.
Table 2. Applications of polysaccharide-based biopolymers in food packaging.
Packaging Material Characteristics of Food
Packaging System Mechanical Properties Thermal Properties Application Reference
Starch
Starch-cinnamon
essential oil
(CEO)—TiO2NPs
•Improved oxygen,
mechanical
properties, and
water vapor
permeability
•Decreased barrier
properties
•Antimicrobial
activity against
E. coli,
S. typhimurium, and
S. aureus
TS (MPa): ~18,
~25(respectively for starch,
starch—5% TiO2—3%
CEO)
EB (%): ~26, ~24
(respectively, for starch,
starch—5% TiO2—3%
CEO)
-
Potential active food
packaging material
for fresh pistachio
packaging
[6]
Foods 2023,12, 2422 13 of 59
Table 2. Cont.
Packaging Material Characteristics of Food
Packaging System Mechanical Properties Thermal Properties Application Reference
Starch—PBAT
•Improved flexibility,
water vapor barrier,
mechanical
properties, and
hydrophobicity
TS (MPa): 1.5, 7.4 MPa
(respectively, for
starch—0% PBAT,
starch—50 wt% PBAT)
EB (%): ~100, ~450
(respectively, for
starch—0% PBAT,
starch—50 wt% PBAT)
-Potential active food
packaging material [9]
Starch—cellulose
nanofibers (CNF)
•Improved water
barrier, optical and
mechanical
TS (MPa): 8.9 ±0.1,
16.5
±
0.4 (respectively, for
starch, starch—10% CNF)
EB (%): 83.2 ±0.7,
13.2 ±1.2(respectively, for
starch, starch—10% CNF
-Potential active food
packaging material [105]
Starch—cellulose
nanocrystals (CNC)
•Improved tensile
strength, Young’s
modulus, and
mechanical
properties.
•Decreased water
vapor permeability
TS (MPa): ~16, ~24
(respectively, for starch,
starch—15% CNC)
EB (%): ~13, ~4
(respectively, for starch,
starch—15% CNC)
Tonset (◦C):
307 ±3.21,
266 ±6.03
(respectively, for
starch, starch—15%
CNC)
Tmax (◦C):
335 ±2.65,
328 ±1.53
(respectively, for
starch, starch—15%
CNC)
Potential active food
packaging material [7]
Starch—ZnO-
rosemary
polyphenols included
in PVA
•Improved Young’s
modulus, stress and
strain at break, and
tensile toughness
•Decreased water
vapor permeability
•Antimicrobial
activity against
E. coli and
antioxidant activity
TS (MPa): 2.1 ±0.2,
3.5 ±0.2 (respectively, for
starch,
starch—ZnO-rosemary
polyphenols included in
PVA)
EB (%): 50 ±16, 76 ±9
(respectively, for starch,
starch–ZnO-rosemary
polyphenols included
in PVA)
-Potential active food
packaging material [8]
Starch—cellulose
nanofiber
(CNF)-thymol
•Improved the water
vapor barrier
•Tensile strength and
Young’s modulus
decreased, and the
elongation at break
increased with
increasing thymol
concentration
•
Antibacterial activity
against E. coli
TS (MPa): ~11, ~6
(respectively, for
starch—CNF,
starch—CNF-10% thymol)
EB (%): ~110, ~122
(respectively, for
starch—CNF,
starch—CNF-10% thymol)
-Potential active food
packaging material [106]
Cassava starch—red
cabbage extract
•
Colorimetric reaction
to pH change (2–12)
and volatile
ammonia visible
with the naked eye
TS (MPa): 5.73 ±0.12,
10.37 ±0.22 (respectively,
for native cassava starch,
oxidized-acetylated starch)
EB (%): 102.44 ±3.2,
60.52 ±3.39 (respectively,
for native cassava starch,
oxidized-acetylated starch)
Weight losses of the
first phase (30–105
◦
C), the second phase
(106–320 ◦C), and
the third phase
(above 320 ◦C)
Potential intelligent
food packaging
material.
[107]
Chitosan
Chitosan—polyvinyl
alcohol-
anthocyanins
•Improved tensile
strength,
hydrophobic and
barrier properties
- -
Potential intelligent
food packaging
material for real-time
shrimp freshness
monitoring
[109]
Foods 2023,12, 2422 14 of 59
Table 2. Cont.
Packaging Material Characteristics of Food
Packaging System Mechanical Properties Thermal Properties Application Reference
Chitosan—cellulose
acetate
phthalate—ZnO NPs
•Improved thermal
stability and barrier
properties
•Reduced water
contact angle.
Biodegradation of 30
to 50% of film in
28 days
TS (MPa): 8.29 ±0.16,
9.83 ±0.19 (respectively,
for chitosan,
chitosan—cellulose acetate
phthalate—ZnO NPs)
EB (%): 12.67 ±0.38,
15.44 ±0.46 (respectively,
for chitosan,
chitosan—cellulose acetate
phthalate—ZnO NPs)
-
Potential active food
packaging material
for black grapefruits
by increasing
shelf-life up to 9 days
[110]
Chitosan—TiO2NPs
•Exhibit
photodegradation
activity when
exposed to UV light,
thus delaying
ripening process and
changes in quality of
tomatoes
TS (MPa): 10.96 ±1.57,
16.43 ±0.46 (respectively,
for chitosan,
chitosan—TiO2NPs)
EB (%): 57.71 ±1.28
53.06 ±2.15 (respectively,
for chitosan,
chitosan—TiO2NPs)
-
Potential active food
packaging material to
maintain quality and
extend storage life of
climacteric fruit
[111]
Chitosan—TiO2
NPs—Cymbopogon
citratus essential oil
•Incorporation of
TiO2NPs increased
water vapor
permeability and
tensile strength.
•Decreased
elongation at break
and film solubility
TS (MPa): 37.50 ±0.00,
62.46 ±0.13 (respectively,
for chitosan,
chitosan—1%TiO2
NPs—0.5% Cymbopogon
citratus essential oil)
EB (%): 4.77 ±0.03,
4.81 ±0.01 (respectively,
for chitosan,
chitosan—1%TiO2
NPs—0.5% Cymbopogon
citratus essential oil)
-
Potential active
packaging material
for prolong shelf-life
of minced meat by
reducing microbial
growth
[112]
Chitosan—graphene
oxide NPs
•Improved tensile
strength, Young’s
modulus, and
antimicrobial
activity
•Decreased water
vapor permeability
TS (MPa): 0.063 ±0.0041,
0.083 ±0.0034
(respectively, for chitosan,
chitosan—graphene
oxide NPs)
EB (%): 6.45 ±0.05,
6.95 ±0.72 (respectively,
for chitosan,
chitosan—graphene
oxide NPs)
-
Potential active food
packaging bag for
prolonging shelf-life
of melon fruits
[12]
Chitosan-pullulan—
clove-essential-oil-
loaded
chitosan–ZnO hybrid
NPs
•Increased tensile
strength,
hydrophobicity, UV
light blocking ability,
water vapor barrier
and oxygen barrier
properties
•Enhanced
antioxidant activity
•
Antibacterial activity
against P. aeruginosa,
S. aureus, and E. coli
•Extend the shelf-life
of chicken meat by
up to 5 days
TS (MPa): 62.0 ±0.2,
83.7 ±0.2 (respectively,
for chitosan,
chitosan-pullulan—clove-
essential-oil-loaded
chitosan—3% ZnO
hybrid NPs)
EB (%): 5.0
±
0.1, 5.1
±
0.5
(respectively, for chitosan,
chitosan-pullulan—clove-
essential-oil-loaded
chitosan—3% ZnO
hybrid NPs)
-
Potential active
packaging material
for prolonging
shelf-life of chicken
[113]
Chitosan—modified
silica NPs
•Improved
mechanical, water
vapor barrier, and
UV light barrier
properties
•Increased
antioxidant activity
TS (MPa): 101.29 ±0.57,
125.25 ±0.36 (respectively,
for chitosan, chitosan—4%
modified silica NPs)
EB (%): 4.78 ±0.06,
2.26 ±0.11 (respectively,
for chitosan, chitosan—4%
modified silica NPs
Potential antioxidant
active packaging
material
[114]
Foods 2023,12, 2422 15 of 59
Table 2. Cont.
Packaging Material Characteristics of Food
Packaging System Mechanical Properties Thermal Properties Application Reference
Chitosan-alginate—
TiO2
NPs
•Improved
mechanical, UV
barrier, antibacterial,
and biodegradability
properties
•
antimicrobial activity
against foodborne
pathogens E. coli,
S. aureus,S. typhi,
and L. monocytogene
TS (MPa): 1.82 ±0.16,
26.86 ±0.28 (respectively,
for chitosan—alginate,
chitosan-alginate—0.2%
TiO2NPs)
EB (%): 2.05 ±0.64,
3.66 ±0.63 (respectively,
for chitosan –alginate,
chitosan-alginate—0.2%
TiO2NPs)
The first stage of
weight loss is the
temperature range of
60–180 ◦C
The second stage of
weight loss takes
place in the
temperature range of
210–400 ◦C
Potential active food
packaging bag for
prolonging shelf-life
of cherry tomatoes
[29]
Carrageenan
Carrageenan—CuS
NPs
•Improved
mechanical and
thermal properties
•Antimicrobial
activity against
E. coli and
S. aureus
TS (MPa): ~60, ~62
(respectively, for
carrageenan,
carrageenan—0.15%
CuS NPs
EB (%): ~35,
~45(respectively, for
carrageenan,
carrageenan—0.15%
CuS NPs
First step occurred at
about 60–110 ◦C
The second stage
from 120 to 220 ◦C
The third stage, from
230 to 290 ◦C
Potential
antimicrobial active
food packaging
material for beef
packaging
[115]
κ-carrageenan—
Zataria multiflora
extract—nanoclay
•Improved UV
barrier, mechanical
and thermal
properties
•Antimicrobial
activity against
E. coli and
P. aeruginosa
TS (MPa): 17.0 ±2.0,
33.7
±
3.9 (respectively, for
κ-carrageenan-nanoclay,
κ-carrageenan-Zataria
multiflora
extract—nanoclay)
EB (%): 63.8 ±16.8,
20.9
±
5.7 (respectively, for
κ-carrageenan-nanoclay,
κ-carrageenan- Zataria
multiflora
extract—nanoclay)
Initial step of weight
loss around
40–120 ◦C
The second step
around 120–260 ◦C
The third weight loss
stage from
260 to 500 ◦C
Potential active food
packaging material [16]
κ-carrageenan—
pomegranate flesh
and peel extracts
•Improved tensile
strength, water
vapor, and UV light
barrier properties
•High antioxidant,
antimicrobial, and
pH-sensitive
properties
TS (MPa): 24.73 ±1.25,
30.94 ±0.85 (respectively,
for κ-carrageenan,
κ-carrageenan—
pomegranate flesh and
peel extracts)
EB (%): 13.82 ±2.45,
22.29 ±1.54 (respectively,
for κ-carrageenan,
κ-carrageenan—
pomegranate flesh and
peel extracts)
-
Potential active
intelligent food
packaging material
[116]
κ-carrageenan—
cassava
starch
•Improved thermal
and mechanical
properties
•High stiffness and
water solubility
•
Low swelling degree
and water vapor
permeability
TS (MPa): 19.23 ±3.58,
25.88 ±2.55 (respectively,
for 100% κ-carrageenan,
75%
κ-carrageenan—cassava
starch)
EB (%): 4.36 ±0.90,
8.41 ±1.71 (respectively,
for 100% κ-carrageenan,
75%
κ-carrageenan—cassava
starch)
Inflection points in
DTG curves for the
κ-carrageenan
(210 ◦C) and starch
(334 ◦C) films
Potential active food
packaging material [13]
Foods 2023,12, 2422 16 of 59
Table 2. Cont.
Packaging Material Characteristics of Food
Packaging System Mechanical Properties Thermal Properties Application Reference
κ-carrageenan—
cellulose
nanocrystals
•Improved
mechanical, water,
and UV barrier
properties and
thermal stability
TS (MPa): 38.33 ±3.79,
52.73 ±0.70 (respectively,
for κ-carrageenan,
κ-carrageenan—7%
cellulose nanocrystals)
EB (%): 21.50 ±3.72,
25.83 ±2.61 (respectively,
for κ-carrageenan,
κ-carrageenan—7%
cellulose nanocrystals)
The first degradation,
which occurred at
30–200 ◦C
The second
degradation at
230–400 ◦C
Potential active food
packaging material [117]
κ-carrageenan-
gelatin—TiO2
NPs—anthocyanin
•Improved
mechanical
properties and
moisture resistance
•Changes in the
freshness of the fish
samples caused the
films to change color
TS (MPa): 53.9 ±0.6,
23.6
±
2.2 (respectively for
3% κ-carrageenan-gelatin,
3% κ-carrageenan-
gelatin—3% TiO2
NPs—anthocyanin)
EB (%): 1.47 ±0.05,
30.4
±
0.2 (respectively, for
3% κ-carrageenan-gelatin,
3% κ-carrageenan-gelatin-
3% TiO2
NPs—anthocyanin)
The first degradation
170–200 ◦C
Second degradation
around 230–250 ◦C
Third degradation
around 460–480 ◦C
Potential smart and
active packaging
material
[118]
κ-carrageenan—
honey bee pollen
phenolic compounds
•Increased physical
properties and
hydrophilicity
•Increased
antioxidant and
antiradical activity
TS (MPa): 24.60 ±1.65,
35.97 ±0.95 (respectively,
for κ-carrageenan,
κ
-carrageenan—honey bee
pollen phenolic
compounds)
EB (%): 69.91 ±1.75,
78.64 ±2.08 (respectively,
for κ-carrageenan,
κ-carrageenan—honey
bee pollen
phenolic compounds)
T
Onset
: 348
◦
C, 348
◦
C
(respectively, for
κ-carrageenan, κ-
carrageenan—honey
bee pollen
phenolic compounds)
Potential edible films
for beef [119]
Cellulose
Carboxymethyl
cellulose—chitosan—
ZnO
NPs
•Reduced water
vapor permeability
and increased
antimicrobial
activity
- -
Potential active food
packaging material
for bread by reducing
microbial growth
[18]
Carboxymethyl
cellulose—
guanidinylated
chitosan enriched
with TiO2NPs
•Improved thermal
stability, mechanical,
and UV barrier
properties and
antimicrobial
activity
TS (MPa): 25.12 ±1.43,
29.36 ±1.88 (respectively,
for carboxymethyl
cellulose, carboxymethyl
cellulose—guanidinylated
chitosan enriched with 5%
TiO2NPs)
EB (%): (respectively, for
carboxymethyl cellulose,
carboxymethyl
cellulose—guanidinylated
chitosan enriched with 5%
TiO2NPs)
The first
mass loss around
100 ◦C
The second mass loss
of ca. occurred at
216–326 ◦C
The third mass
loss around 600 ◦C
Potential active food
packaging material
for excellent
resistance to mass
loss and spoilage of
green bell pepper
[20]
Foods 2023,12, 2422 17 of 59
Table 2. Cont.
Packaging Material Characteristics of Food
Packaging System Mechanical Properties Thermal Properties Application Reference
Methylcellulose—
jambolão (Syzygium
cumini) skins extract
•Improved
mechanical and
barrier performance
•Biodegradation of
film in sea water in
2 days and soil in
15 days
TS (MPa): 16.10 ±1.52,
21.4 ±1.55 (respectively,
for methylcellulose,
methylcellulose film—50%
jambolão extract)
EB (%): 14.2 ±2.0,
37.5
±
2.0 (respectively, for
methylcellulose,
methylcellulose film—50%
jambolão extract)
Tg (◦C): 166.07,
135.97 (respectively,
for methylcellulose,
methyl-cellulose
film—50%
jambolão extract)
Tm (◦C): 174.37,
161.46 (respectively,
for methylcelllose,
methyl-cellulose
film—50% jambolão
extract)
Potential active
intelligent food
packaging for meat
and aquatic products,
where lipid oxidation
occurs, and the pH
modification is
associated with
food spoilage
[120]
Carboxymethyl
cellulose
(CMC)-starch
•Improved
mechanical
properties, and
water vapor barrier
with the addition of
CMC.
•Slight reduction in
the thermal stability
TS (MPa): 50.2 ±6.9,
32.6
±
2.1 (respectively, for
CMC, 80% CMC-20%
starch)
EB (%): 7.6 ±2.2,
21.2
±
4.3 (respectively, for
CMC, 80% CMC-20%
starch)
The first degradation
at approximately
95 ◦C
The second step of
the thermal occurs
between 145 ◦C and
160 ◦C.
The third stage
occurred in the range
of 250–350 ◦C
Potential active food
packaging material [121]
Cellulose—ZnO NPs
•Improved UV and
oxygen barrier
properties, thermal
stability, and
crystallinity
•Increased
antimicrobial
properties for
B. cereus,S. aureus,
L. monocytogenes,
E. coli,
S. typhimurium, and
V. parahaemolyticus
TS (MPa): 141.70 ±3.70,
126.61 ±15.34
(respectively, for cellulose,
cellulose—1% ZnO NPs)
EB (%): 3.05 ±0.34,
2.58 ±0.73 (respectively,
for cellulose,
cellulose—1% ZnO NPs)
Minor weight loss of
cellulose films at
50–55 ◦C
Depending on the
concentration of
ZnONP, the thermal
degradation was
observed in the range
of 270–330 ◦C
Potential
antimicrobial food
packaging material
[122]
Bacterial cellulose
(BC)-carboxymethyl
cellulose
(CMC)-yeast
•High water
solubility
•
antimicrobial activity
against E. coli,P.
aeruginosa, and S.
aureus
•Enhanced shelf-life
of orange and
tomato coatings
TS (MPa): 17.02 ±1.19,
2.23 ±0.33 (respectively,
for BC, BC-CNC-yeast)
EB (%): 4.77 ±0.56,
15.53 ±0.84 (respectively,
for BC, BC-CNC-yeast)
BC-CNC-yeast first
degradation step at
90 ◦C
BC first degradation
step at 100 ◦C
Second degradation
step for
BC-CNC-yeast
started between
240 ◦C to 260 ◦C and
continued until
330 ◦C
BC cellulose skeleton
degrades up to
300 ◦C
Potential edible food
packaging materials [123]
Agar
Agar—melanin NPs
•Improved
UV-blocking,
hydrophobicity,
mechanical, water
vapor barrier
properties, and
antioxidant activity
TS (MPa): 34.8 ±0.7,
46.7
±
1.7 (respectively, for
agar, agar—0.5% melanin
NPs)
EB (%): 11.8 ±0.7,
12.2
±
0.9 (respectively, for
agar, agar—0.5%
melanin NPs)
Initial weight loss at
60–110 ◦C
The next weight loss
started at around
200 ◦C
The maximum
weight loss at 250 ◦C
Potential antioxidant
active food
packaging material
[21]
Foods 2023,12, 2422 18 of 59
Table 2. Cont.
Packaging Material Characteristics of Food
Packaging System Mechanical Properties Thermal Properties Application Reference
Agar—thermoplastic
corn starch—glycerol
•Improved barrier,
tensile properties,
and light
transmittance
•Decreased water
permeability and
solubility
TS (MPa): 1.8 ±0.2,
10.7
±
2.1 (respectively, for
thermoplastic corn starch,
60% agar—thermoplastic
corn starch)
-Potential active food
packaging material [22]
Agar—grey
triggerfish skin
gelatin—vine leaves
ethanolic extract
•Improved
mechanical
properties, thermal
stability, and
antioxidant activity
TS (MPa): 68.15 ±1.20,
62.50 ±1.10 (respectively,
for gelatin-agar bilayer
and gelatin-agar
bilayer—5 mg/mL vine
leaves)
EB (%): 21.20 ±1.91,
25.20 ±1.10 (respectively,
for gelatin-agar bilayer
and gelatin-agar
bilayer—5 mg/mL
vine leaves)
Tg (◦C): 65.15, 65.24
(respectively, for
gelatin-agar bilayer
and gelatin-agar
bilayer—5 mg/mL
vine leaves)
Potential active food
packaging material [23]
Agar—sodium
alginate-SiO2NPs
•Improved
mechanical
properties, tensile
strength, UV barrier
properties, water
resistance, and
thermal stability
•Low minimum
swelling degree and
water solubility
TS (MPa): 45.18 ±1.34,
74.68 ±2.23 (respectively,
for agar—sodium alginate,
agar—sodium alginate-10
wt% SiO2NPs)
EB (%): 33.04 ±0.40,
52.99 ±1.65 (respectively,
for agar—sodium alginate,
agar—sodium alginate-10
wt% SiO2NPs)
The first step of
weight loss occurred
at 50–150 ◦C
The second stage of
weight loss was
160–310 ◦C
The third step, for
temperature higher
than 310 ◦C
Potential active food
packaging material [3]
Agar—maltodextrin
bees wax
•Improved tensile
strength, Young’s
modulus, contact
angle, surface
hydrophobicity, and
mechanical
properties
•Low water vapor
permeability
TS (MPa): ~20, ~40
(respectively, for
agar—maltodextrin bees
wax, agar—maltodextrin
bees wax-tween 80)
The first endothermic
peak centered at
65 ◦C, the second
melting peaks
around 110 ◦C
Potential active food
packaging material
for higher
water vapor
resistance material
[124]
Agar—AgNPs
•Antimicrobial
activity against
L. monocytogenes and
E. coli
•Color and oxidative
rancidity
preservation of beef
- - Potential active food
packaging material. [125]
Agar—sugarcane
Wax—butterfly pea
flower extract
•Visual color change
in the presence of
ammonia vapors
and pH (2–12)
•Enhanced physical
and mechanical
properties
TS (MPa): 0.412 ±0.016,
1.140 ±0.172 (respectively,
for agar—butterfly pea
flower extract,
agar—sugarcane
wax—butterfly pea flower
extract)
EB (%): 69.000 ±0.091,
46.000 ±0.175
(respectively, for
agar—butterfly pea flower
ex-tract, agar—sugarcane
wax—butterfly pea
flower ex-tract)
Potential intelligent
food packaging
material for optical
tracking of
shrimp freshness
[126]
Foods 2023,12, 2422 19 of 59
Table 2. Cont.
Packaging Material Characteristics of Food
Packaging System Mechanical Properties Thermal Properties Application Reference
Pectin
Pectin–
polycaprolactone
•Improved thermal
stability, mechanical
properties, barrier
properties, and
hydrophobic nature.
EB (%): ~1, ~20
(respectively, for pectin,
pectin–polycaprolactone)
The first one,
centered around
100 ◦C, is due to the
loss of water; the
second between 200
and 400 ◦C is
attributed to the
pyrolytic
decomposition of
macromolecular
chains; and the third
one is between 500
and 700 ◦C
Potential active food
packaging material. [24]
Pectin—copaiba oil
nanoemulsions
•
Improved elongation
at break, and
antimicrobial activity
against S. aureus and
E. coli
TS (MPa): 41.8 ±6.5,
12.4
±
4.7 (respectively, for
pectin, pectin—6% copaiba
oil nanoemulsions)
EB (%): 1.7
±
0.1, 2.4
±
0.5
(respectively, for pectin,
pectin—6% copaiba
oil nanoemulsions)
Tonset (◦C): 215, 200
(respectively, for
pectin, pectin—6%
copaiba
oil nanoemulsions)
Potential active food
packaging material [27]
Pectin—cocoa bean
shell waste extract—
ZnO-Zn-NPs
•Improved thermal,
oxidative stability,
and oxygen barrier
properties
•Decrease in oxygen
transmission rate
-
Tmax (◦C): 231 ±1,
229 ±1 (respectively,
for pectin,
pectin—5% cocoa
bean shell waste
extract—3%
ZnO-Zn-NPs)
Potential active food
packaging material [25]
Pectin—pullulan
•Improved water
vapor barrier, UV
barrier, mechanical
properties, thermal
stability, and surface
hydrophobicity
•Protection against
oxidation for
food preservation
TS (MPa): 19.5 ±2.8,
19.1 ±2.6, 23.2 ±2.4
(respectively, for pectin,
pullulan, 30% pectin-70%
pullulan)
EB (%): 1.8
±
0.3, 4.7
±
0.3,
2.9 ±0.9 (respectively, for
pectin, pullulan, 30%
pectin–70% pullulan)
The first step weight
loss between 60 and
120 ◦C
The second
degradation step in
the temperature
range 150–240 ◦C
The third step of
degradation between
240 and 370 ◦C
Potential active food
packaging material [40]
Pectin-starch—TiO2
NPs
•Improved
mechanical, thermal
stability and
moisture, and UV
barrier properties
•Decreased moisture
content, solubility,
and moisture uptake
TS (MPa): 22.34 ±0.89,
26.16 ±0.16 (respectively,
for pectin-starch,
pectin-starch—TiO2NPs)
EB (%): 12.96 ±0.43, 8.12
±0.94 (respectively, for
pectin-starch,
pectin-starch—TiO2NPs)
Tg (◦C): 63.05 ±1.2,
79.63 ±0.42
(respectively, for
pectin- starch,
pectin-starch—TiO2
NPs)
Tm (◦C):
156.41 ±0.30,
172.33 ±0.65
(respectively for
pectin-starch,
pectin-starch—TiO2
NPs)
Potential edible film [127]
Pectin—kiwifruit
(Actinidia chinensis)
peel extract
•Enhanced tensile
strength and
Young’s modulus
•Increased the
shelf-life of chicken
thigh by lower
degree of lipid
oxidation
TS (MPa): 42.30 ±0.82,
21.65 ±0.97 (respectively,
for pectin, pectin—1.5%
kiwifruit peel extract)
EB (%): 10.77 ±0.70,
20.32 ±1.32 (respectively,
for pectin, pectin-1.5%
kiwifruit peel extract)
Potential active food
packaging material [128]
Foods 2023,12, 2422 20 of 59
Table 2. Cont.
Packaging Material Characteristics of Food
Packaging System Mechanical Properties Thermal Properties Application Reference
Pectin-agar—zinc
sulfide NPs
•Improved
mechanical and UV
barrier properties
•High antibacterial
activity against
E. coli and
L. monocytogenes
TS (MPa): 50.3 ±2.8,
47.4
±
3.2 (respectively, for
pectin-agar,
pectin-agar—zinc sulfide
NPs)
EB (%): 4.7
±
1.5, 9.9
±
2.6
(respectively, for
pec-tin-agar,
pectin-agar—zinc
sulfide NPs)
The first weight loss
occurred at
50–110 ◦C with a
maximum
decomposition
temperature of
55–60 ◦C
The second weight
loss was observed at
115–250 ◦C with a
maximum
decomposition
temperature of
~220 ◦C
The third weight loss
appeared 250–340 ◦C
with a maximum
degradation around
300 ◦C
Potential active food
packaging material [129]
Alginate
Sodium
alginate—oregano
essential oil
•Antimicrobial
activity against
L. monocytogenes - -
Potential edible film
for prolong the
shelf-life of ham
slices by reducing
microbial growth
[32]
Alginate—sepiolite
modified with myrtle
berries extract
•
Improved elongation
at break, tensile
strength, water
vapor, and UV
barrier properties
TS (MPa): 38 ±4, 87 ±8
(respectively, for alginate,
alginate—sepiolite
modified with myrtle
berries extract)
EB (%): 3.8
±
0.9, 5.6
±
0.9
(respectively, for alginate,
alginate—sepiolite
modified with myrtle
berries extract)
The first stage of
weight loss 100 ◦C
The second stage
occurs in the
temperature range of
110–160 ◦C
The third stage
occurs in the
temperature range of
160–366 ◦C
The fourth stage at
temperatures above
366 ◦C
Potential active food
packaging material [28]
Sodium alginate-
carboxymethyl
cellulose—
epigallocatechin
gallate
•Improved
antimicrobial activity
and lipid oxidation
prevention
TS (MPa): 4.28 ±0.69,
10.78 ±2.15 (respectively,
for sodium alginate,
sodium
alginate—carboxymethyl
cellulose—1.6%
epigallocatechin gallate)
EB (%): 27.50 ±2.08,
11.20 ±1.57 (respectively,
for sodium alginate,
sodium
alginate—carboxymethyl
cellulose—1.6%
epigallocatechin gallate)
-
Edible coatings for
prolong the shelf-life
of fresh pork by
reducing lipid
oxidation and
microbial growth
[31]
Sodium
alginate-pectin-citric
acid—tartaric acid
•Improved tensile
strength, chemical
resistivity, and
thermal properties
•Nontoxic and
biodegradable
TS (MPa): 18.38, 17.20
(respectively, for sodium
alginate-citric acid,
pectin—citric acid)
Tonset (
◦
C): 99.8, 99.9
Potential edible
packing film for food
wrapping [130]
Foods 2023,12, 2422 21 of 59
Table 2. Cont.
Packaging Material Characteristics of Food
Packaging System Mechanical Properties Thermal Properties Application Reference
Alginate—Zn-MgO
NPs
•
Antibacterial activity
against
L. monocytogenes
•Moderate
cytotoxicity of MgO
NPs towards
mammalian cells
- -
Extend the shelf-life
of Cold-Smoked
Salmon by
controlling
L. monocytogenes
growth
Potential
antimicrobial active
food packaging
material
[131]
Sodium
alginate-cellulose
nano
whisker—copper
oxide NPs
•
Antibacterial activity
against S. aureus,
Salmonella sp.,
C albicans, and
Trichodenna spp.
•Increased
antioxidant activity
- -
Prevent microbial
contamination in
fresh cut pepper
Potential active food
packaging material
[132]
Alginate—aloe
vera–garlic oil
•Enhanced thermal
and mechanical
properties
•
Increased UV barrier
properties and
antimicrobial
properties
•Enhanced shelf-life
of coated tomato
TS (MPa): 17 ±0.71, 21.85
±1.22 (respectively, for
alginate, alginate—2%
aloe vera–5% garlic oil)
EB (%): 10 ±0.91,
41.55 ±0.64 (respectively,
for alginate, alginate—2%
aloe vera–5% garlic oil)
The first stage of
mass loss around
100 ◦C
The second step of
mass loss at 218 ◦C
The 3rd stage of mass
loss at 266 ◦C
Edible coating
for tomato [133]
Alginate—sulfur NPs
•Enhance mechanical
and water vapor
barrier properties
•Antimicrobial
activity against
L. monocytogenes
TS (MPa): 58.5 ±0.8, 63.8
±1.2 (respectively, for
alginate, alginate—3%
sulfur NPs)
EB (%): 7.5
±
0.1, 6.8
±
0.9
(respectively, for alginate,
alginate—3% sulfur NPs)
The initial weight
loss of up to 100 ◦C
The second step
degradation occurred
between 200 and
300 ◦C
Potential active food
packaging material [134]
Gums
Gellan
gum—xanthan
gum-zinc oxide NPs
•Improved tensile
strength, thermal
stability, and water
and UV barrier
properties
•Decreased contact
angle and water
vapor permeability
TS (MPa): 22.1 ±0.9,
35.5
±
1.2 (respectively, for
gellan gum—xanthan
gum, gellan
gum—xanthan gum-5 wt%
zinc oxide NPs)
EB (%): 30.0 ±1.5,
25.1
±
1.1 (respectively, for
gellan gum—xanthan
gum, gellan
gum—xanthan gum-5 wt%
zinc oxide NPs)
Tg (◦C): 69.9 ±0.4,
74.8 ±0.9
(respectively, for
gellan gum—xanthan
gum, gellan
gum—xanthan
gum-5 wt% zinc
oxide NPs)
Tm (◦C): 217.0 ±0.3,
219.3 ±0.4
(respectively for
gellan gum—xanthan
gum, gellan
gum—xanthan
gum-5 wt% zinc
oxide NPs)
Potential active food
packaging material [34]
Xanthan
gum—PVA-red grape
pomace
•Improved
mechanical strength,
antioxidant and
antimicrobial activity
- - Potential active food
packaging material [33]
Foods 2023,12, 2422 22 of 59
Table 2. Cont.
Packaging Material Characteristics of Food
Packaging System Mechanical Properties Thermal Properties Application Reference
Xanthan—curdlan
•Improved tensile
strength, water
solubility,
mechanical, and
moisture barrier
properties
TS (MPa): ~16, ~14, ~28
(respectively, for curdlan,
xanthan, 50% xanthan-50%
curdlan)
EB (%): ~25, ~7, ~17
(respectively, for curdlan,
xanthan, 50% xanthan-50%
curdlan)
The first weight loss
observed between
86.5 and 104.33 ◦C
The maximum
weight loss was
observed between
294.3 and 319.04 ◦C
Potential active food
packaging material [135]
Gellan gum—purple
sweet potato
anthocyanins
•Improved
mechanical
properties,
water-resistant and
antioxidant activity
•Reduced
hydrophilicity,
swelling properties,
and water vapor
transmission rates
TS (MPa): 1.2 ±0.2,
8.9 ±1.1 (respectively, for
gellan gum, gellan
gum—purple sweet potato
anthocyanins)
EB (%): 1.5
±
0.9, 4.3
±
1.2
(respectively, for gellan
gum, gellan gum—purple
sweet potato
anthocyanins)
-
Potential intelligent
food packaging
material to detect the
spoilage of
protein-rich foods
caused by
bacteria growth
[136]
Gellan gum—agar-
montmorillonite
•Improved thermal
stability, tensile
strength, and
rheological
properties.
Decreased water
barrier properties
and contact angle
TS (MPa): 29.9 ±1.2,
44.0
±
1.4 (respectively, for
gellan gum— agar, gellan
gum—agar-10%
montmorillonite)
EB (%): 29.5 ±0.9,
19.9
±
0.8 (respectively, for
gellan gum—-agar, gellan
gum—agar-10%
montmorillonite)
Tg (◦C): 70.2 ±0.4,
77.1 ±0.8
(respectively, for
gellan gum—agar,
gellan
gum—agar-10%
montmorillonite)
Tm (◦C): 198.4 ±0.3,
214.2 ±0.5
(respectively, for
gellan gum—agar,
gellan
gum—agar-10%
montmorillonite)
Potential active food
packaging material [87]
Tragacanth
gum—PVA gallic
acid
•Improved tensile
properties and water
vapor transmission
rate
•Enhanced
hydrophobicity and
thermal stability
TS (MPa): 15.3 ±2.1, 45.7
±1.4 (respectively for
PVA, tragacanth
gum—PVA gallic acid)
EB (%): 149.3 ±16.2,
69.4 ±25.1 (respectively,
for PVA, tragacanth
gum—PVA gallic acid)
Tg (◦C): 43.3, 70.5
(respectively, for PVA,
tragacanth
gum—PVA gallic
acid)
Tm (◦C): 192.7, 216.3
(respectively, for PVA,
tragacanth
gum—PVA
gallic acid)
Potential active food
packaging material [137]
Lignin
Lignin—gellan
gum-hydroxyethyl
cellulose
•Improved thermal,
mechanical,
hydrophobic, and
UV barrier
properties and
antioxidant activity
•Showed
non-cytotoxic
activities and
antimicrobial
activity
TS (MPa): 23.0 ±1.1, 39.0
±0.8 (respectively, for
gellan gum, lignin—gellan
gum-hydroxyethyl
cellulose)
EB (%): 20.3 ±0.4,
32.5
±
0.4 (respectively, for
gellan gum, lignin—gellan
gum-hydroxyethyl
cellulose)
Tg (◦C): 149.2 ±0.5,
156.9 ±0.3
(respectively, for
gellan gum,
lignin—gellan
gum-hydroxyethyl
cellulose)
Tm (◦C): 205.6 ±0.6,
216.0 ±0.3
(respectively, for
gellan gum,
lignin—gellan
gum-hydroxyethyl
cellulose)
Potential active food
packaging material [93]
Foods 2023,12, 2422 23 of 59
Table 2. Cont.
Packaging Material Characteristics of Food
Packaging System Mechanical Properties Thermal Properties Application Reference
Alkali lignin-
lignosulfonate—soy
protein isolate
•Improved
mechanical, UV
barrier, and thermal
properties
•Decreased water
vapor permeability
TS (MPa): 4.74 ±0.34,
8.01 ±0.89, 10.98 ±1.02
(respectively, for soy
protein, 10%
lignosulfonate–soy
protein, 10% alkali
lignin—soy protein)
EB (%): 126.33 ±17.9,
79.95 ±5.32, 7.45 ±1.24
(respectively, for soy
protein, 10%
lignosulfonate—soy
protein, 10% alkali
lignin—soy protein)
The first weight loss
50–100 ◦C.
The second weight
loss occurred at
around
300 ◦C
Potential active food
packaging material [36]
Lignin—
nanocellulose
•Enhanced oxygen
permeability and UV
barrier properties
- - Potential active food
packaging material [37]
Lignin—poly(lactic
acid)
•Enhanced
mechanical and
thermal properties
•Good antioxidant
activity
TS (MPa): ~40, ~30
(respectively, for PLA,
PLA—40% lignin)
EB (%): ~15, ~2
(respectively, for PLA,
PLA—40% lignin)
Tonset (◦C): 323.6,
306.1 (respectively,
for PLA, PLA—40%
lignin)
Tmax (◦C): 330.2,
320.7 (respectively,
for PLA, PLA—40%
lignin)
Potential active food
packaging material [38]
Pullulan
Pullulan-tempo
cellulose nanofibrils—
montmorillonite
clay
•Improved tensile
strength, thermal
stability, and water
barrier properties
and decreased
moisture
susceptibility
TS (MPa): ~35, ~5
(respectively, for pullulan,
pullulan-tempo cellulose
nanofibrils—5%
montmorillonite clay)
Maximum
decomposition
temperature for
pullulan and
pullulan-tempo
cellulose nanofibrils—
montmorillonite clay
film were around
98 ◦C and 308.27 ◦C
Potential active food
packaging material [39]
Pullulan—lysozyme
nanofibers
•Improved
mechanical
properties, thermal
stability, and
antioxidant activity
•
Antibacterial activity
against S. aureus and
lysozyme-resistant
bacteria
TS (MPa): 35.0 ±4.4,
37.6 ±2.2 (respectively,
pullulan, pullulan—5%
lysozyme nanofibers)
EB (%): 6.63 ±1.11,
1.84 ±0.29 (respectively,
pullulan, pullulan—5%
lysozyme nanofibers)
Pullulan has a single
weight loss step with
initial and maximum
decomposition
temperatures of 250
and 300 ◦C
Lysozyme nanofibers
has a single-step
degradation profile
with maximum
degradation
temperature of
308 ◦C
Potential edible films
for active packaging [138]
Pullulan—egg white
•Improved
mechanical
properties
•Film showed lower
degradation speed
TS (MPa): 60.65, 329.48
(respectively, for pullulan,
pullulan—egg white)
EB (%): 1.43, 10.33
(respectively, for pullulan,
pullulan—egg white)
Initial loss at 100 ◦C
Final weight loss step
at 270–450 ◦C
Potential edible films
for active packaging [139]
Foods 2023,12, 2422 24 of 59
Table 2. Cont.
Packaging Material Characteristics of Food
Packaging System Mechanical Properties Thermal Properties Application Reference
Pullulan-graphene—
nanocellulose
•Increased opacity,
hydrophobicity,
tensile strength,
oxygen transmission
rate, and water
vapor transmission
rate
•
Antibacterial activity
against E. coli and
S. aureus
TS (MPa): ~7, ~20
(respectively, for
pullulan—nanocellulose,
pullulan-graphene—
nanocellulose
-Potential active food
packaging material [140]
Pullulan-curcumin—
Ag
NPs
•Maintained the
textural and
physicochemical
broiler meat for
14 days of storage
attributes along with
minimal oxidative
rancidity
- - Potential active food
packaging material [141]
Pullulan-
carboxylated
cellulose
nanocrystal-tea
polyphenol
•Enhanced water
barrier properties,
thermal stability, and
tensile strength
•
Improved UV barrier
properties,
antioxidant activity,
and antimicrobial
activity
TS (MPa): 25.28 ±1.21,
34.49 ±1.32 (respectively,
for pullulan-carboxylated
cellulose nanocrystal,
pullulan-carboxylated
cellulose nanocrystal-5%
tea polyphenol)
EB (%): 8.67 ±0.54,
5.76 ±0.25 (respectively,
for pullulan-carboxylated
cellulose nanocrystal,
pullulan-carboxylated
cellulose nanocrystal-5%
tea polyphenol)
The first step of
thermal degradation
was 80–150 ◦C
Maximum
decomposition
temperature at
around 230–400 ◦C
Potential active food
packaging material [142]
Pullulan-chitin
nanofbers-
curcumin—
anthocyanins
•Antioxidant and
antimicrobial
activities
•Color change with
pH
TS (MPa): 23.95 ±5.57,
10.18 ±4.37 (respectively,
for pullulan,
pullulan-chitin nanofibers-
curcumin—anthocyanins)
EB (%): 7.45 ±2.66,
10.05 ±6.83 (respectively,
for pullulan,
pullulan-chitin nanofibers-
curcumin—anthocyanins)
Significant weight
loss at temperatures
between 250 and
400 ◦C
Potential active and
intelligent food
packaging material
[143]
Pullulan—propolis
extract
•
Improved UV barrier
and decreased
transparency
•Enhanced
antimicrobial activity
mainly against yeast
TS (MPa): 24.62 ±2.12,
14.42 ±1.99 (respectively,
for pullulan,
pullulan—propolis extract)
EB (%): 21.00 ±0.92,
15.92 ±1.51 (respectively,
for pullulan,
pullulan—propolis
extract)
-Potential active food
packaging material [144]
Curdlan
Curdlan—PVA-
thyme essential
oil
•
Improved elongation
at break, antioxidant
activity, and
antibacterial activity
•Decrease in water
vapor permeability
was lower
TS (MPa): ~9, ~12
(respectively, for curdlan,
4curdlan—1PVA-thyme
essential oil)
EB (%): ~90, ~180
(respectively, for curdlan,
4curdlan—1PVA-thyme
essential oil)
The heat absorption
peak of curdlan film
is 309 ◦C
When PVA is added,
the heat absorption
peak conversion
temperature of the
film is up
to 342 ◦C
Increased shelf-life of
chilled meat up to
10 days
Potential active food
packaging material.
[41]
Foods 2023,12, 2422 25 of 59
Table 2. Cont.
Packaging Material Characteristics of Food
Packaging System Mechanical Properties Thermal Properties Application Reference
Curdlan-Xanthan
•High mechanical
and moisture barrier
properties was
observed in the
blend films with 5:5
and 4:6 ratios of
xanthan and curdlan
TS (MPa): ~16, ~14, ~28
(respectively, for curdlan,
xanthan, 50% xanthan-50%
curdlan)
EB (%): preparation of a
novel curdlan/bacterial
cellulose/cinnamon
essential oil blending film
for food packaging
application 25, ~7, ~17
(respectively, for curdlan,
xanthan, 50% xanthan-50%
curdlan)
The first weight loss
observed between
86.5 and 104.33 ◦C
The maximum
weight loss was
observed between
294.3 and 319.04 ◦C
Potential active food
packaging material [135]
Curdlan-bacterial
cellulose-cinnamon
essential oil
•Enhanced tensile
strength, the
crystallinity, and the
thermal stability
•Reduced water
vapor permeability,
moisture content,
and the lightness
•Good antibacterial
activity and
antioxidant capacity
TS (MPa): ~5, ~7
(respectively, for curdlan,
curdlan-2% bacterial
celllose-15% cinnamon
essential oil)
EB (%): ~70, ~80
(respectively, for curdlan,
curdlan-2% bacterial
celllose-15% cinnamon
essential oil)
The first heat
absorption peak of
the films was
observed around
40–110 ◦C
Exothermic peak of
curdlan films are
around 270–300 ◦C
Exothermic peaks of
blending film were
around 285 ◦C and
282 ◦C
Potential active food
packaging material [42]
The incorporation of NPs such as cellulose nanofibers, [
105
] cellulose nanocrystals [
7
],
and ZnO [
8
] also improves the properties of starch. Tibolla et al. [
105
] developed a bio-
nanocomposite film by using cellulose nanofibers isolated from the unripe banana peel
by acid hydrolysis as reinforcement agents in a matrix of banana starch. The cellulose
nanofibers incorporated into starch films showed high elongation at break (30.6%), good
tensile strength (12.3 MPa), low moisture (13.66%), solubility in water (24.1%), and in-
ferior UV/light transmission. Coelho et al. [
7
] formed a bio-nanocomposite film by em-
bedding pomace pre-treated cellulose nanocrystals into a starch matrix by casting tech-
nique. The incorporation of cellulose nanocrystals reduced the water vapor permeability
of the starch films from 7.5
±
0.35 g
×
h
·
m
·
Pa
−1
to 4.25 (1% cellulose nanocrystals) and
4.55 ×10−7g×h·m·Pa−1
(1% cellulose nanocrystals). Films containing 5 to 15% cellulose
nanocrystals were more opaque and degraded faster when exposed to light, while the
mechanical, and barrier properties were unaffected.
The combination of cinnamon essential oil and TiO
2
NPs was incorporated into a Sago
starch matrix to form packaging for fresh pistachios [
6
]. The addition of essential oil into
the starch matrix enhanced the permeability of starch films to oxygen and water vapor,
while increasing the concentration of TiO
2
NPs lowered the barrier properties. Further, the
moisture content of starch films was reduced from 12.96% to 8.04%, and water solubility
declined from 25% to 13.7%. Starch-based films have been developed to become smart
packaging systems along with antioxidant activity and color changes at different pH as
for the study by Ceballos et al. [
145
] on yerba mate extract. Extrusion and compression
molding were used to make native or hydrolyzed starch and yerba mate extract films. The
developed film was hydrophobic with an increased plasticizer effect and disintegrated after
10 weeks of soil burial.
In the recent study of Li et al. [
82
] lactic acid bacteria (probiotic) and sodium car-
boxymethyl cellulose were incorporated into starch to form an edible film. To boost the
film’s probiotic activity, two lactic acid bacteria species (Lactiplantibacillus plantarum and
Pediococcus pentosaceus) with high exopolysaccharide yield were used from a pickled water
sample. The composite film’s antioxidant activity was greatly increased, with the highest
Foods 2023,12, 2422 26 of 59
activity of 48.1%. The water vapor and light transmission of the film were reduced, thus
resulting in lipid oxidation deterioration and leading to increased shelf-life of banana.
6.1.2. Chitosan
Chitosan is a nontoxic, biodegradable polycationic copolymer derived from chitin by
deacetylation. It is insoluble in water and organic solvents but forms polycations in media
with a pH less than 6.5. Chitosan is a highly researched biodegradable biopolymer due to
its attractive properties, which include biocompatibility, film-forming ability, antioxidant
activity, antimicrobial activity, mechanical properties, selective permeability to CO
2
and
O
2
, UV barrier properties, good optical properties, transparency, flexibility, and fat and
oil resistance. A chitosan-based packaging system increases the emulsifying effect, the
natural flavor, the texture setting, the deacidification, and the color stabilization of food
products, thereby enhancing their quality, safety, and shelf-life. However, the limitation of
pure chitosan in food packaging is found to be weakened water vapor barrier properties;
thus, it is highly sensitive to moisture, and a film developed from chitosan is found to be
brittle with low elasticity [4,10,96,109,110,146].
Chitosan has been blended with many biopolymers in studies to increase the relevant
properties. The non-covalent bond formation between chitosan and alginate makes them
one of the most compatible biopolymers for food packaging [
147
], while starch–chitosan
is also considered a promising blend film [
148
]. Further, polymer blends with pectin
make packaging material transparent with increased mechanical properties [
149
]. Some
studies in recent years have demonstrated that the addition of NPs to the chitosan matrix
increases the antimicrobial properties of the film while prolonging the shelf-life of the food
product. A study by Kaewklin, Siripatrawan, and Suwanagul [
111
] shows that TiO
2
NPs
exhibited ethylene photodegradation while delaying the ripening process and enhancing
the quality of the tomatoes. In this study, TiO
2
NPs were incorporated into a chitosan matrix
to form a packaging film. Paiva et al. [
12
] reinforced graphene oxide NPs into chitosan
to form packaging bags by the solvent casting method. The film decreased water vapor
permeability and increased tensile strength and Young’s modulus while prolonging the
shelf-life of melon fruits.
To overcome the shortfalls of the pure chitosan natural plant extracts such as olive
pomace [
150
], purple-fleshed sweet potato extract [
151
], apple peel [
152
], black soybean
seed coat extract [
153
], and Chinese chive root extract [
154
] have been used, which exhibit
good antioxidant and antimicrobial activity. Further, some of these plant extracts (soybean
seed coat extract and purple-fleshed sweet potato extract) were studied for pH-sensing
ability, thus forming a smart food packing material.
Glycerol/sorbitol is added to the chitosan matrix as plasticizers making the film
less soluble in water, with increased optical property and less brittleness [
10
,
155
] Further,
studies have been conducted using a combination of other biopolymers, NPs, and plant
extracts together on the chitosan matrix. Jha [
10
] developed a packaging material with the
combination of chitosan–starch–nanoclay and different ratios of grapefruit seed extract.
The film containing 1.5% grapefruit seed extract showed increased mechanical (tensile
strength of 19.6 MPa and 55.8% elongation at break), thermal, and water barrier properties.
Further, this film showed a higher zone of inhibition against A. niger and high antifungal
activity in stored bread at 25
◦
C for 20 days. Lin et al. [
156
] developed a functional food
packaging material of chitosan–nano-silicon aerogel films incorporated with Okara powder
by the casting method as shown in Figure 4. The produced films in general had increased
flexibility, while the increased chitosan concentration of the film resulted in increased
tensile strength. Further, the increased chitosan content led to a significant decrease in the
water contact angle. The film also showed strong antibacterial activity against E. coli and
S. aureus.
Foods 2023,12, 2422 27 of 59
2
Figure 4.
Development of chitosan–nano-silicon aerogel films incorporated with Okara powder by
casting method. Reprinted/adapted with permission from Ref. [156]. 2020, Elsevier.
Further, a chitosan-based food packaging system with NPs was formed by Panariello,
Coltelli, and Buchignani [
157
] with the incorporation of nanostructured chitin and cellulose.
Here, chitosan and nanostructured chitin-based films were prepared in combination with
cellulose by using the solution casting method.
6.1.3. Carrageenan
Carrageenan is a linear, sulfated water-soluble polysaccharide that is extracted from
red seaweeds belonging to the Rhodophyceae family [
4
,
95
]. It is widely used as a food addi-
tive. The commercial production of
κ
-carrageenan developed by CP Kelco is GENUGEL
®
,
which is used as a thickening, stabilizing, gelling, and texturizing agent in food appli-
cations [
13
]. Carrageenan has a scope as a food packaging material due to its excel-
lent film-forming ability, thermal stability, antibacterial properties, barrier properties,
and biodegradability. However, it has limited application due to undesirable mechan-
ical and water resistance properties [
102
]. The addition of other polysaccharides such
as starch [
14
] significantly increases the physical, thermal, and mechanical properties
of the film. Further to their studies, Sun et al. [
158
] designed an antioxidant and pH-
responsive
κ
-Carrageenan-hydroxypropyl methylcellulose film with the incorporation
Foods 2023,12, 2422 28 of 59
of Prunus maackii juice. With the increasing Prunus maackii concentration, antioxidant
activity reached 28.76%, and elongation at break was 48.64%. The lowest oxygen per-
meability was
1.63 cm3mm m−2day−1atm−1
, and the least water vapor permeability
was
0.37 ±0.01 g m−1s−1Pa−1×10−12
. When the volatile base nitrogen content in the
pork was 19.26 mg/100 g, the film turned from red to blue, indicating the monitoring of
pork freshness.
Recently, further studies have been conducted using carrageenan biopolymer and
nanofillers—carrageenan-CuSNPs [
115
],
κ
-carrageenan-Zataria multifloraextract—nanoclay [
16
],
and
κ
-carrageenan-glycerol-cellulose nanocrystals [
117
]. Nanoclay, 1–3% v/vZataria mul-
tiflora plant extract, and glycerol as a plasticizer were used to develop a biodegradable
carrageenan nanocomposite film by using two different methods (adding glycerol before
the formation of film-forming solution and after film-forming solution formation) [
16
].
The addition of glycerol to the carrageenan solution before the film formation solution
increased tensile strength by 56% while lowering elongation at the break by 61%. All films
were effective against E. coli and P. aeruginosa.
Additionally, Liu et al. [
116
] developed an active intelligent food packaging material
using
κ
-carrageenan with the incorporation of pomegranate flesh or peel extracts. The
incorporation of pomegranate flesh and or peel extracts enhanced the tensile strength from
24.73 MPa (pure
κ
-carrageenan film) to a maximum of 30.94 MPa and reduced water vapor
permeability from 8.32
×
10
−11
g m
−1
s
−1
Pa
−1
(pure
κ
-carrageenan film) to a minimum
of 3.47
×
10
−11
g m
−1
s
−1
Pa
−1
. Furthermore, due to the abundance of anthocyanins,
pomegranate-flesh-extract-containing films demonstrated pH-sensitive properties.
To develop a less expensive film, semi-refined carrageenan has been produced. How-
ever, they have poor water vapor permeability and relatively poor mechanical properties.
Due to its inferior optical properties, it can be used for packaging applications such as
food containers and cups. The mechanical and water barrier properties of semi-refined
carrageenan film samples can be enhanced by photo-crosslinking with UV light to produce
a low-cost food packaging material [17].
6.1.4. Cellulose
Cellulose is the most abundant natural organic compound widely present in plants
and bacteria. Cellulose is the agro-industrial waste that is mostly reused. The cellulose
molecule (C
6
H
10
O
5
) n) has a linear ribbon-like conformation, and its compounds are bound
together by the so-called
β
1-4, glycosidic bonds. It is widely used as raw materials for
biodegradable films and edible films that are renewable, low cost, nontoxicity, biocompat-
ible, biodegradable, odorless, tasteless, and chemically stable. Further, it has increased
oxygen, hydrocarbon barrier properties, and water vapor permeability [91].
The most used cellulose derivatives in food packaging are methylcellulose (MC), hy-
droxypropyl methylcellulose (HPMC), hydroxypropyl cellulose (HPC), and carboxymethyl
cellulose (CMC); however, due to their hydrophilic nature, they have poor water vapor
barriers. In addition to the above demerits, cellulose has low mechanical strength and has
opacity [17,30,121].
As per the study of Tavares et al. [
121
], they formed films through the solvent casting
method by increasing the carboxymethyl cellulose concentration to form a neat starch film.
There was an increase in the mechanical (elastic modulus was 14.5 times higher) and water
vapor barrier properties of films by reducing the water vapor permeability by 56% (40%
carboxymethyl cellulose incorporated film). However, there is a slight reduction in thermal
stability from 294
◦
C for the pure starch film to 253
◦
C for the 40% carboxymethyl cellulose
incorporated film [
159
]. Further, studies were carried out on carboxymethyl cellulose
by [
120
] where glycerol, mucilage from Dioscorea opposita, and Ag NPs were incorporated
into a carboxymethyl cellulose matrix by the casting method. With the decreasing concen-
trations of carboxymethyl cellulose in the film, tensile strength reduced from 18.30 MPa
to 6.78 MPa, while the elongation at break increased from 38.52% to 62.33%. The water
Foods 2023,12, 2422 29 of 59
vapor permeability reduced from 25.06 g
·
mm/m
2·
d
·
kPa to 19.87 g
·
mm/m
2·
d
·
kPa. The
film showed significant antibacterial activity against S. aureus and E. coli.
A pH-sensitive active film was produced from methylcellulose with the incorpora-
tion of anthocyanins present in jambolão (Syzygium cumini) skin by the casting technique.
When compared to the pure methylcellulose film, the tensile strength improved from
16.10 MPa to 21.4 MPa (methylcellulose film + 50% jambolão extract), while elongation
at break increased from 14.2% to 37.5% (methylcellulose film + 50% jambolão extract).
As a result of the pH-sensitive structure of anthocyanins, color variations were observed
in films when the pH was altered. Methylcellulose exhibited no radical scavenging ac-
tivity, whereas increasing concentrations of jambolão jambolo extract increased radical
scavenging activity. The films biodegraded in 2 days in sea water and 15 days in soil [
120
].
Additionally, studies have also been performed with the addition of a nanofiller to a cel-
lulose matrix; examples are cellulose-lignin-cellulose nanocrystals [
160
], carboxymethyl
cellulose-chitosan-ZnO NPs [
18
], and carboxymethyl cellulose-guanidinylated chitosan
enriched with TiO
2
NPs [
20
]. These packaging materials are considered potential active
packaging materials with improved thermal stability, mechanical and UV barrier properties,
and antimicrobial activity.
6.1.5. Agar
Agar is a heterogeneous gelatinous polysaccharide extracted from marine red algae.
The agar chain consists of D-galactopyranose and 3,6-anhydro-L-galactopyranose with
alternating (1, 4) and (1, 3) linkages. Agar is insoluble in cold water and soluble in hot water,
while it is stable in a different environment with low pH and high temperature [
22
,
87
]. It is
used as a biodegradable film in food packaging because of its desirable film-forming ability,
nontoxicity, stability in different environmental conditions, continuity, and transparency.
However, its application in food packaging is limited due to poor water vapor barrier
properties, mechanical properties, brittleness, thermal stability, and strong hydrophilic
characteristics [
4
,
21
,
23
,
87
,
92
]. A considerable amount of research has been conducted on
applications of agar in food packaging by the incorporation of reinforcement agents, for
example, nanomaterials, other biopolymers, plasticizers, or antimicrobial agents.
The incorporation of other polymers such as maltodextrin–beeswax–liquid paraf-
fin [
124
], maltodextrin–beeswax [
161
], starch [
22
], and gelatin [
23
] considerably increase
the properties of agar. Fekete et al. [
22
] developed agar-based packaging films by casting
or melt blending with a high glycerol concentration after agar was added to thermoplastic
corn starch in a high concentration. The addition of agar to the starch matrix significantly
increased the stiffness and strength of the film. Further, young’s modulus and tensile
strength increased with the increasing concentrations of agar. Zhang et al. [
161
] developed
an agar–maltodextrin–beeswax pseudo-bilayer edible film with different homogenizing
speeds for mixing. The film was homogenized at a speed of 8000 rpm for 1 min and had
the maximum tensile strength (20.57 MPa), young’s modulus (640.60 MPa), and contact
angle (92.9◦) and the minimum water vapor permeability (2.18 ×10−12 g m−1s−1Pa−1).
Melanin NPs [
21
], sodium alginate-nano-SiO
2
[
3
], and montmorillonite-gellan gum [
93
]
all improve the UV-blocking activity, hydrophobicity, mechanical properties, water vapor
barrier, and thermal stability of agar, which makes them effective materials for food pack-
ing. Roy and Rhim [
21
] utilized melanin NPs isolated from sepia ink as the reinforcement
agent for an agar-based packaging film. There was a decrease in the UV and visible light
transmittance in the agar–melanin NPs film when compared to the pure agar film. The
tensile strength (from 34.8 MPa to 39.8 MPa) and elongation at break (from 11.8% to 16.1%)
of agar increased when 0.25% of melanin NPs was added. Lee et al. [
87
] combined an-
other biopolymer gellan gum and montmorillonite nanoclay into an agar matrix to form
a ternary nanocomposite film via the solution casting method. This film had improved
thermal stability (119.4–174.7
◦
C) and tensile strength (29.9–44 MPa) upon the addition
of montmorillonite. Furthermore, there was a decrease in the water barrier (1.9–1.7) and
contact angle (56.8–49.4◦) upon the incorporation of the montmorillonite nanoclay.
Foods 2023,12, 2422 30 of 59
6.1.6. Pectin
Pectin is a natural, renewable, and abundant polysaccharide in plant cell walls consist-
ing of
α
(1–4) galacturonic acid monomers with different degrees of esterification [
24
]. It is
an acid and water-soluble polymer that is used in industry as a stabilizing thickening, encap-
sulating, and gelling agent. Pectin’s beneficial characteristics, such as being biodegradable,
renewable, cheap, gas permeable, and film-forming, make it a good material for edible
films, biodegradable films, or gels used in food packing. However, pectin has certain char-
acteristics that are not beneficial, such as negative mechanical properties, brittleness, low
thermal stability, high solubility in water, and no antimicrobial properties [
24
,
26
,
40
,
95
,
127
].
Priyadarshi, Kim, and Rhim, [
40
] developed a hybrid biopolymer active food packag-
ing material, pectin–pullulan, with different ratios of polymers through the solution casting
method. The blend with the 50:50 ratio of pectin and pulullan exhibited the highest thermal
stability, surface hydrophobicity, smallest water contact angle of 63.4
◦
, and oil absorption
value of 6.33 g m−2.
The thermal and oxidative stability and oxygen barrier properties of pectin have been
improved by the addition of nanofillers into the matrix pectin–cocoa bean shell waste
extract–ZnO-Zn-NPs [
25
]. Dash, Ali, and Das [
127
] also developed an edible film with
lemon-waste pectin and sweet potato starch with TiO
2
NPs by using the casting method.
The film exhibited improved mechanical (tensile strength increased from 22.34 MPa to
26.16 MPa), moisture barrier, and UV barrier properties with the addition of TiO2NPs. In
recent years, studies have been performed on pectin modification such as pectin chemically
modified with polycaprolactone, which reduces pectin’s hydrophilicity [
24
], pectin films
activated by copaiba oil nanoemulsions that improve physicomechanical and antimicrobial
properties [
27
], and thermoplastic pectin, which increases water resistance and mechanical
properties [26].
6.1.7. Alginate
Alginate is a natural polysaccharide extracted from brown algae, consisting of a
(1–4) chain of a-L-guluronate and R-D-mannuronate. Alginate is regarded as a food safety
additive by the FDA (US Food and Drug Administration) and EFSA (European Food
Safety Authority). Commercially, alginate is used as a thickener, stabilizer, and gelling
agent in foods such as deserts, sauces, and beverages [
162
]. Alginate can produce a strong
insoluble polymer that has improved water barrier properties, mechanical properties, co-
hesiveness, stiffness, flavor maintenance, and slower fat oxidation. It has poor moisture
barriers, and its hygroscopicity slows the dehydration of food [
30
,
95
]. Alginate is brittle,
has poor water resistance, and is easily dissolved in water at room temperature [
3
]. Alginate
packaging materials have been modified in recent years with the addition of other biopoly-
mers such as sodium alginate–carboxymethyl cellulose–epigallocatechin gallate [
31
], and
sodium alginate–pectin–citric acid–tartaric acid [
130
]; active agents such as sodium alginate–
oregano essential oil [
32
] and alginate–sepiolite modified with myrtle berries extract [
28
];
and nanofillers such as alginate-Zn-MgO NPs [
131
] and sodium alginate-cellulose nano
whisker-CuO NPs [
132
]. Singh et al. [
130
] developed a pectin (extracted from the waste
pineapple shell)–sodium alginate (extracted from seaweed)-based film by crosslinking with
citric acid and tartaric acid. The film was found to be a suitable edible packaging material
through the studies of mice feed, plant growth substrate, and vermicomposting. Cheikh
et al. [
28
] utilized the solution casting to make alginate nanocomposite films comprising
sepiolite modified with polyphenol-rich myrtle berry extract. When compared to the
control film, the hybrid films improved elongation at break (from 3.8% to 5.6%), tensile
strength (from 38 MPa to 87 MPa), water vapor, and UV barrier properties. The films’
antioxidant activity was greatly improved and boosted as the myrtle berry extract content
was increased.
Foods 2023,12, 2422 31 of 59
6.1.8. Gums
Gums are polysaccharides found in microbial production with a few different types.
Arabic gums are found in the stems of various Acacia species, and it shows excellent
film-forming ability, encapsulation properties, and unique emulsification. Xanthan gum
is an exopolysaccharide synthesized by Xanthomonas campestris. Xanthan gum is used as
a food stabilizer, thickener, and emulsifier. It forms a stable viscous solution in hot/cold
water at different ranges of temperature and pH [
95
]. Gellan is a polysaccharide produced
by Sphingomonas elodea. Gellan is used as a gelling agent, texturizer, and carrier for food
additives in the food industry [
95
]. Gum biopolymers have a controlled viscosity, good bio-
compatibility, and low cytotoxicity. However, it has limited application in food packaging
due to the high cost of production and low rheological, mechanical, and barrier proper-
ties. Recently, studies of xanthan gum biopolymers have been performed in developing
xanthan gum–polyvinyl alcohol (PVA)-red grape pomace [
33
] and xanthan–curdlan [
135
]
packaging materials, which were able to improve mechanical strength and antioxidant and
antimicrobial activity. Lee et al. [
87
] developed ternary composite films from gellan gum–
agar–montmorillonite via the solution casting method. The incorporated montmorillonite
was able to improve thermal stability by 46.3%, tensile strength by 47.1%, and rheological
properties. Further studies on the gellan gum intelligent food packaging material were
performed by Wei et al. [
136
], which improved mechanical properties, water resistance, and
antioxidant activity with the potential to detect the spoilage of protein-rich foods caused by
bacteria growth. Finally, the studies of Rukmanikrishnan, Ismail, and Manoharan [
34
] were
performed with the combination of two gum biopolymers and a nanofiller—gellan gum–
xanthan gum–zinc oxide NPs—by using a solvent evaporation method. This combination
improved tensile strength by 60.6%, thermal stability, and UV barrier properties. The water
vapor permeability decreased by 39.7%, while moisture content values decreased by 38.0%.
6.1.9. Lignin
Lignin is a complex phenolic compound that is abundantly found in the plant cell
wall. It has good antioxidant properties and is a natural UV blocker. However, lignin has
low mechanical and barrier properties. The combination with agar enhances the water
vapor barrier and mechanical and thermal stability of the film while reducing the swelling
ratio, transparency, and moisture content [
4
,
160
]. Limited studies have been performed
on lignin biopolymers where lignin is combined with other biopolymers; lignin–gellan
gum–hydroxyethyl cellulose [
93
] and alkali lignin–lignosulfonate–soy protein isolate [
36
]
were tested to improve their UV barrier properties. Rukmanikrishnan, et al. [
93
] used the
solvent casting process to make composite films using gellan gum, hydroxyethyl cellulose,
and lignin (0, 1, 5, and 10 wt%). The addition of 10 wt% lignin increased the tensile strength
of the film by 59.2%. This film showed 100% protection against UVB and 90% protection
against UVA. The UV barrier properties of lignin were also observed in the studies of
Zadeh, O’Keefe, and Kim [
36
] examining an alkali lignin–lignosulfonate–soy protein isolate
film. Moreover, this film showed increased mechanical and thermal stability.
6.1.10. Pullulan
Pullulan is a natural and biocompatible microbial polymer obtained from Aureoba-
sidium pullulans. It has an alternation of
α
-(1,4) and
α
-(1,6) glycosidic bonds. Pullulan
is currently used as a low-calorie component in food, coagulating agents, coating and
wrapping material, and binders for fertilizers. It has many beneficial characteristics that can
be used in food packaging such as being biodegradable, nontoxic, odorless, colorless, heat-
sealable, water permeable, transparent, low in oxygen, oil permeable, and flexible. Further,
it is also palatable and water-soluble, making it a suitable edible film material. However,
it has high moisture sensitivity, affecting food packaging performance, in addition to low
mechanical properties and brittleness [40,113].
The undesirable properties of pullulan were overcome in the study of Yeasmin
et al. [
39
] by the addition of montmorillonite and tempo cellulose nanofibrils to a pul-
Foods 2023,12, 2422 32 of 59
lulan matrix. This film showed great optical transparency, moisture resistance, tensile
strength (the highest 45.9 MPa was observed for 5 wt.% montmorillonite-containing films),
and thermal properties. In addition to this study, Silva, Vilela, and Almeida [
138
] also
developed a packaging material with pullulan–lysozyme nanofibers by a simple solvent
casting technique from aqueous suspensions. This film showed improved mechanical
properties (young’s modulus = 1.91–2.50 GPa), thermal stability, 77% DPPH scavenging
activity, and antimicrobial properties. Studies on a potential edible film from pullulan—egg
white were performed by Han, Liu, and Liu [139].
6.1.11. Curdlan
Curdlan is nontoxic, biodegradable, colorless, odourless, has a high absorption/retention
of moisture, can withstand extreme cold conditions, is insoluble in water, and is thermally
stable. Nonetheless, it possesses weak mechanical properties. Studies of curdlan are
extremely limited in food packaging applications, although it can be used as a suitable
copolymer due to its characteristics. Zhang et al. [
41
] developed a packaging material based
on curdlan-PVA-thyme essential oil. The curdlan: PVA film ratio of 4:1 had the highest
tensile strength of 11.81 MPa and an elongation at break of 189.31%. The antioxidant
properties of the film were improved by the addition of thyme essential oil, and the shelf-
life of chilled meat was extended up to 10 days.
6.2. Protein-Based Biopolymers
Protein biopolymers are made up of amino acid copolymers and can be divided into
plant-origin proteins (e.g., gluten and soy) and animal-origin proteins (e.g., whey, collagen,
and keratin). Protein biopolymers have many beneficial properties such as good mechanical
properties, excellent gas barrier properties, good film-forming ability, nutritional value,
and elasticity, thus making them suitable for food packaging applications. However, these
proteins are hydrophilic, making them have poor water barrier properties. Protein-based
biopolymers have potential applications in biomedicine and food packaging. Protein-based
polymers including whey protein, gelatin, wheat gluten, corn, zein, and soy protein have
been used to produce edible films in food packaging, improving their mechanical and
barrier properties. Further, biopolymers such as keratin, casein, zein, gelatin, and soy
protein play an important role in the preparation of various industrial products such as
shopping bags, protection film, and sanitary products. The mechanical properties and
other properties of protein biopolymers can be further enhanced by blending them with
other biopolymers (protein/non-protein) or with other reinforcement agents as shown in
Table 3[
55
]. The mechanical properties of some of the studies depicted in Table 3have
been taken, and a scatter plot has been drawn for a better understanding of the properties,
which can be seen in Figure 5. Protein biopolymers act as coating films in food packaging.
WHEYLAYER and THERMOWHEY are European initiatives designed to develop coatings
based on protein biopolymers. These initiatives developed oxygen barrier coatings for
reusable multilayer packaging materials as an alternative to synthetic polymers [77].
6.2.1. Whey Protein
Whey protein is a byproduct of the manufacturing of cheese. It is inexpensive, abun-
dant, biodegradable, nutritious, film-forming, nutrient-rich, and has gas barrier properties.
However, it has poor tensile strength and moisture resistance. Recent studies have been
conducted in blended biopolymers such as whey protein–furcellaran–yerba mate–white tea
extracts [
52
]. The incorporation of nanofiller such as whey protein–corn oil-TiO
2
NPs [
50
]
and whey protein–chitosan nanofiber–nano-formulated cinnamon oil [
163
] has also been
examined. Finally, the incorporation of active agents such as whey protein–nanoemulsions
of orange peel (Citrus sinensis) essential oil has been studied [51].
Foods 2023,12, 2422 33 of 59
3
Figure 5.
Elongation at break versus tensile strength for protein-based biopolymers. Abbreviation:
Ker—Keratin, Col—collagen, LEO—lemon essential oil, Ch—chitosan, WP—whey protein, CO—
corn oil, Gel—gelatin, PP—pomegranate peel extract, EP—Epigallocatechin gallate and laminated
with PLA.
Pluta-Kubica et al. [
52
] developed a whey protein films–furcellaran-based edible film
with the incorporation of yerba mate and white tea extracts by using the casting method as
shown in Figure 6. The permeability of water vapor, water content, solubility, modulus
elasticity, and thermal stability of the film were all increased by yerba mate. During storage,
the water content and activity of cheese packed in each type of biopolymer film reduced
along with the coliform total bacterial count. Montes-de-Oca-Ávalos et al. [
50
] developed a
TiO
2
NPs-incorporated corn oil–whey protein-based edible film with varying concentrations
of whey proteins. The TiO
2
NPS-loaded bio-nanocomposite film had the highest elastic
modulus (19.2 MPa), Young’s modulus (19.4 MPa), and elongation at break (119%).
3
Figure 6.
Development of whey protein–furcellaran-based edible film with the incorporation of yerba
mate and white tea extracts [52]. Reprinted/adapted with permission from Ref. [52]. 2020, Elsevier.
Foods 2023,12, 2422 34 of 59
6.2.2. Gelatin
Gelatin is a renewable, sustainable protein source that is mostly found in the skin and
bones of an animal. Collagen, in its natural form, has little use for application. Therefore,
one chooses to extract the gelatin present in its composition for use. To obtain the gelatin,
it is necessary for the collagen to undergo a hydrolysis process (acidic, alkaline, or enzy-
matic), associated with high temperatures to break the covalent bonds, releasing the gelatin
molecules through denaturation of the helix triple. After cooling the solution, the chains
absorb the water, forming gelatin. The two types of collagen (A and B) can be obtained
from partial hydrolysis or thermal degradation of collagen. It is currently used in the food,
pharmaceutical, and photographic industries due to its nontoxicity, renewability, biodegrad-
ability, and excellent film-forming ability. Furthermore, gelatin is biocompatible, adhesive,
abundantly available, flexible, and transparent. It also is cheaper to manufacture while
it has excellent water, aroma, and oxygen barrier properties. However, it is not suitable
as a food packaging material alone due to its poor mechanical properties and processabil-
ity [
4
,
23
,
43
,
44
]. Recent research has examined the blending of different biopolymers, such
as Gelatin–PLA [
43
], Gelatin–chitosan-3-phenylacetic acid [
164
], and Gelatin–agar bilayer
vine leaves [
23
]. The studies of Nilsuwan, Guerrero, and Caba [
43
] focused on developing a
bilayer fish gelatin film incorporated with epigallocatechin gallate and laminated with PLA
by thermo-compression molding. These films had high lipid oxidation retardation ability
and thus can be used for the packaging of high-lipid-content foods. Ge et al. [
165
] also
developed a green nanocomposite film with pH sensitivity and antioxidant activity using
gelatin–chitin nanocrystals–anthocyanins that can be used for the freshness monitoring of
high-protein foods. In addition, the bio-nanocomposite Gelatin–grapefruit seed-TiO
2
NPs
was developed by Riahi et al. [
44
] via the solution casting method. The film had improved
mechanical properties, water contact angle, and antimicrobial and antioxidant activity,
while it prevented UV light transmission completely.
6.2.3. Soy Proteins
Soy proteins are abundant, renewable, and highly biodegradable proteins. Soy pro-
teins consist of a high amount of polar amino acids such as cystine, arginine, lysine, and
histidine. Thus, it has improved the mechanical strength, oxygen and lipid barrier, high
water vapor permeability, and thermal properties in addition to flexibility, low cost, sustain-
ability, biocompatibility, film-forming capacity, smoothness, and transparency. However,
soy proteins have low water resistance, low thermoplasticity, brittleness, low mechan-
ical properties, low film gloss, and low tensile strength. Soy proteins are available in
three types—soy flour, soy protein concentrate, and soy protein isolate. Soya protein
isolates are easily biodegradable but have poor plasticity, brittleness, and water vapor
permeability [46,95].
6.2.4. Zein
Zein is the main protein of corn endosperm and the chief byproduct of the bioethanol
industry. It is a polyamine that has a high content of hydrophobic amino acids. Zein is
soluble in ethanol and insoluble in water. Zein has great qualities for film-forming in
the food packaging industry, such as hydrophobicity, antimicrobial potential, antioxidant
activity, adhesive film-forming ability, and extreme resistance to moisture and oxygen.
Further, Zein is also considered a safe material for the food system by the Food and Drug
Administration (FDA). However, it breaks easily and has poor processability, mechanical
properties, elongation at break, and thermal properties. Thus, it is unable to be used as a
packaging material in its pure form. Plasticizers such as linoleic acid, palmitic acid, oleic
acid, poly (ethylene glycol) (PEG), poly (propylene glycol) (PPG), poly (tetramethylene
glycol) (PTMG), and glycerol has been added to zein films to increase brittleness, elasticity,
and flexibility [
46
,
95
]. Recently, the properties of zein proteins have been enhanced by
combining polymer blends and nanoparticles; studies have shown that the following
combinations improve the properties: Zein–potato starch–chitosan NPs incorporated with
Foods 2023,12, 2422 35 of 59
curcumin [
166
], zein–chitosan–cinnamodendron dinisii Schwanke essential oil [
55
], zein–
sodium alginate-TiO
2
NPs-betanin [
56
], zein–pomegranate peel extract–chitosan NPs [
167
],
and zein-TiO
2
nanofibers [
54
]. Xin et al. [
166
] developed a zein–starch-based film with
the incorporation of curcumin-loaded chitosan NPs by using the solution casting method.
The highest tensile strength (13.1 MPa) and elongation at break (50.3%) were observed in
the films with the lowest zein concentration (30%). These films were able to prolong the
Schizothorax prenati fillets’ shelf-life up to 15 days. On the other hand, Amjadi, Almasi,
and Ghorbani [
56
] used electrospinning technology to create novel nanofibers based on
zein–sodium alginate integrated with TiO
2
NPs and betanin for food packaging. The
film showed acceptable mechanical properties, high surface hydrophobicity, and a DPPH
scavenging activity of 64.42%. It also showed antimicrobial activity against S. aureus and
E. coli.
6.2.5. Keratin
Keratin is a natural protein found in bird feathers, wool, or other natural resources.
Keratin is a biodegradable, biocompatible, and hydrophobic compound with greater ab-
sorption properties. However, keratin has very poor mechanical properties, making it
not a suitable packaging material to be used in its pure form [
168
]. A limited number of
studies have been performed on keratin-based food packaging materials. In recent years,
Ramirez et al. [
58
] developed a keratin–citric acid-based food packaging material by using
the casting method. This film showed an improved biocidal effect and a 600% elongation
at the break. It can prolong the shelf-life of carrots when compared to commercial film.
Further, Ramakrishnan et al. [
59
] also designed a keratin–glycerol-based biodegradable
packaging material from keratin extracted from chicken feathers. The best mechanical and
thermal properties are found in keratin films with 2% glycerol. Biodegradability tests have
shown that all produced bioplastics films are biodegradable.
6.2.6. Collagen
Collagen is a naturally abundant, biocompatible, and biodegradable protein found in
animals. It is industrially produced from the skin and bones of swine, cattle, and fish skin.
Collagen has a great film-forming ability, antioxidant properties, moisture and oxygen bar-
rier, and structural integrity. However, its high water vapor transmission rates and poor me-
chanical properties give collagen limited applications in the food packaging industry. Thus,
very limited studies have been performed on collagen food packaging [
169
]. Jiang et al. [
60
]
fabricated a food packaging material with a collagen matrix by using the solvent casting
method, where the chitosan–lemon essential oil NPs were incorporated. The film had im-
proved tensile strength, elongation at break from 65.41% to 104.34% (30% chitosan–lemon
essential oil NPs), and reduced oxygen permeability from
0.57 cm3mm m−2d−1kPa−1
to
0.39 cm
3
mm m
−2
d
−1
kPa
−1
(30% chitosan–lemon essential oil NPs). With regard to the
shelf-life study, when the pork was stored at 4
◦
C for 21 days, films significantly prevented
lipid oxidation, reduced microbial multiplication, and prolonged the deterioration of pork.
6.3. Aliphatic Polyesters
Aliphatic polyesters are biopolymers composed of repeating structures that, upon
degradation, produce metabolites such as poly(beta-hydroxy alkanoate)s and poly(alpha-
hydroxy alkanoate)s. They are easily biodegradable because of the presence of ester bonds
in the soft chains making them sensitive to hydrolysis. Aliphatic polyesters have been
used as commercial products as an alternative to synthetic properties due to their similar
properties; however, they lack mechanical and thermal properties [
92
]. Some of the aliphatic
polyesters that are used in food packaging are PLA, PBAT, polyhydroxyalkanoate (PHA),
polybutylene succinate (PBS), polyhydroxybutyrate (PHB), and polycaprolactone (PCL),
and their properties are shown in Table 4. The mechanical properties of some of the
studies depicted in Table 4have been taken, and a scatter plot has been drawn for a better
understanding of the properties, which can be seen in Figure 7.
Foods 2023,12, 2422 36 of 59
4
Figure 7.
Elongation at break versus tensile strength for aliphatic polyester biopolymers. Abbre-
viation: CNC—cellulose nanocrystals, GTE—green tea extract, TA—tannic acid, GA—gallic acid,
FA—ferulic acid.
Aliphatic polyesters amount for most of the bioplastics, which amount to 2.11 million
tonnes of global production in 2020, out of which the highest market segment is the
packaging market, which accounts for 47% (0.99 million tonnes). As for the European
Bioplastic [
78
] PBAT, PLA, PBS, and PHA are currently in use in the rigid and flexible
packaging marketing sector.
6.3.1. Poly Lactic Acid (PLA)
Poly lactic acid (PLA) has become one of the most significant commercial polymers that
are biodegradable and bio-based thermoplastics. PLA is made up of alpha-hydroxy acids,
which include polyglycolic acid or polymandelic. PLA is derived by depolymerization
of the lactic acid monomer obtained from sugar cane, corn starch, or tapioca. Compa-
nies such as Ingeo (Nature Works, Plymouth, MN, USA), PURAC (PURAC Co., Rayong,
Thailand), BIOFRONT (Teijin, Tokyo, Japan), HiSun (Revoda, Stoney Creek, ON, Canada),
and Pyramid (Tate and Lyle, Pinckneyville, Denmark) manufacture biodegradable PLA
films. These produced biopolymers are used in a wide variety of industrial applications
such as disposable household items (drinking cups, cutlery, trays, food plates, and food
containers), food packaging, waste bags, shopping bags, agriculture (soil retention sheeting
and agriculture films), drug delivery systems, biomedical devices disposable garments,
feminine hygiene products, and diapers [
77
]. PLA is used in commercial food packaging for
manufacturing caps (PLA blends), coffee capsules/pouches (PLA/PHB), shopping/waste
bags (Blends of PLA/PHA/PBAT), clear films for fruits and vegetables (PLA/Blends of
PLA/Bio-PET), and teabags (PLA blends) [170].
Foods 2023,12, 2422 37 of 59
Table 3. Applications of protein biopolymers in food packaging.
Packaging Material Characteristics of Food
Packaging System Mechanical Properties Thermal Properties Application Reference
Gelatin
Gelatin-grapefruit
seed (GSE)—TiO2
NPs
•Improved
mechanical
properties, water
contact angle, and
antioxidant activity
•Decreased water
vapor permeability
and UV light
transmittance.
•
Antibacterial activity
against E. coli and
L. monocytogenes
TS (MPa): 60.6 ±1.1,
57.9 ±1.3, 63.4 ±1.5,
61.5 ±1.7, 58.3 ±1.9,
55.2 ±1.6 Gel,
(respectively for Gel/GSE,
Gel/GSE/0.5%TiO2,
Gel/GSE/1%TiO2,
Gel/GSE/2%TiO2,
Gel/GSE/5%TiO2)
EB (%)10.6 ±0.8,
12.7 ±1.2, 9.6 ±1.7,
10.4 ±2.0, 12.5 ±1.1,
13.3
±
1.9 (respectively, for
Gel/GSE,
Gel/GSE/0.5%TiO2,
Gel/GSE/1%TiO2,
Gel/GSE/2%TiO2,
Gel/GSE/5%TiO2)
Initial weight loss at
80–120 ◦C,
subsequent
degradation varied
between 200 and
300
◦
C, and third step
of weight loss
around 320 ◦C
Potential active food
packaging material [44]
Gelatin—PLA
•Improved
mechanical and
UV–visible light
barrier properties
•Low water vapor
and oxygen
permeability
TS (MPa): 24.90 ±5.59,
31.21 ±2.88 (respectively,
for Gelatin-PLA and
Epigallocatechin gallate,
laminated with PLA and
emulsified with gelatin)
EB (%): 8.27 ±3.26,
11.83 ±3.05 (respectively,
for Gelatin-PLA and
Epigallo-catechin gallate,
laminated with PLA and
emulsified with gelatin)
-
Control lipid
oxidation and
increased shelf-life of
fried salmon skins up
to 30 days. Suitable
active packaging
material for
high-lipid-content
foods.
[43]
Gelatin-chitosan-3-
phenylacetic
acid
•Improved thermal
stability, water
stability, and water
vapor permeability
•Antimicrobial
activity against
S. enterica and
S. aureus
The first weight loss
occurred around
75–150 ◦C
A major loss occurred
at 200–300 ◦C
Potential active food
packaging material [164]
Gelatin-agar
bilayer—vine leaves
•Improved
mechanical
properties and
antioxidant and
amicrobial activity
TS (MPa): 68.15 ±1.20,
62.50 ±1.10 (respectively,
for Gelatin-agar bilayer
and Gelatin-agar
bilayer—5 mg/mL
vine leaves)
EB (%): 21.20 ±1.91,
25.20 ±1.10 (respectively,
for Gelatin-agar bilayer
and Gelatin-agar
bilayer—5 mg/mL
vine leaves)
Tg (◦C): 65.15, 65.24
(respectively, for
Gelatin-agar bilayer
and Gelatin-agar
bilayer—5 mg/mL
vine leaves)
Potential active food
packaging material [23]
Gelatin-oxidized
chitin nanocrystals
(Ch)—black rice bran
anthocyanins
(BACNs)
•Improved UV–vis
light barrier and
antioxidant activity
TS: 9.44
±
0.29, 2.53
±
0.12
(respectively, for
BACNs-Ch0 and
BACNs-Ch100)
EB (%): 115.33 ±3.06,
141.67 ±3.06 (respectively,
for BACNs-Ch0 and
BACNs-Ch100)
-
Monitor the freshness
of shrimp and hairtail
by visible color
changes. Potential
intelligent packaging
material for freshness
monitoring of high
protein foods
[165]
Foods 2023,12, 2422 38 of 59
Table 3. Cont.
Packaging Material Characteristics of Food
Packaging System Mechanical Properties Thermal Properties Application Reference
Gelatin-
carrageenan—carbon
dots
•Enhanced
mechanical
properties
•High antioxidant
activity
TS (MPa): 52.8 ±6.3,
81.2
±
5.3 (respectively, for
gelatin-carrageenan and
gelatin-carrageenan-10%
carbon dots)
EB (%): 3.9
±
1.1, 6.4
±
0.6
(respectively, for
gelatin-carrageenan and
gelatin-carrageenan—10%
carbon dots)
The first weight loss
at 55−110 ◦C
The second thermal
degradation from
125 ◦C to 280 ◦C
The third thermal
degradation from
285 ◦C to 350 ◦C
Potential active food
packaging material [171]
Gelatin-carrageenan-
shikonin—propolis
•Excellent pH (2–12)
responsive
color-changing
properties
•
Enhanced UV barrier
properties
•Monitored the
freshness of
packaged milk
TS(MPa): 43.9 ±2.3,
41.7
±
3.0 (respectively, for
Gelatin-Carrageenan and
Gelatin-carrageenan-
shikonin—propolis)
EB (%): 3.2 ±0.2, 3.6 ±0.1
(respectively, for
Gelatin-Carrageenan and
Gelatin-carrageenan-
shikonin—proplis)
Three step
degradation between
290 and 350 ◦C
Potential intelligent
food packaging
material
[172]
Gelatin—tea
polyphenol/ε-poly
(L-lysine)
•
High hydrophobicity
and UV barrier
properties
•Excellent
antibacterial activity
and antioxidant
activity
- - Potential active food
packaging material [173]
Keratins
Keratin—citric acid
•Improved biocidal
effect, elongation
value, and
transparency
TS(MPa): 1.49 ±0.80
EB (%):138 ±21
First stage of weight
loss 60 ◦C for pure
keratin and 80 ◦C for
keratin—citric acid
The second stage at
224 ◦C for pure
keratin and 195 ◦C
for keratin—citric
acid
Increased shelf-life of
carrot. Active
packaging material
suitable for food
preservation
[58]
Keratin—glycerol
•Improved
mechanical and
thermal properties.
•Fully biodegradable
according to
biodegradability test
TS(MPa): 9.59, 0.0409
(respectively, for 15 wt%
glycerol-sugar palm starch
film, 10 wt% keratin
bioplastic film)
-Potential active food
packaging material [168]
Feather
keratin—dialdehyde
carboxymethyl
cellulose
•
Increased UV barrier
properties and
transmittance
•Reduced moisture
sensitivity
TS(MPa): 17.6 ±3.0,
30.8 ±4.6 (respectively,
for keratin,
keratin—dialdehyde
carboxymethyl cellulose)
EB (%): 4.0
±
0.9, 0.7
±
0.4
(respectively, for keratin,
keratin—dialdehyde
carboxymethyl cellulose)
-Potential edible food
packaging material [59]
Keratin—starch
•Improved
mechanical
properties
•decayed over 20% of
the original mass
after 12 days of
soil burial
TS(MPa): 8.3 ±0.2,
13.8
±
0.2 (respectively, for
starch-keratin 20:0,
starch-keratin 20:5)
EB (%): 19.7 ±0.1,
33.3 ±0 (respectively, for
starch-keratin 20:0,
starch-keratin 20:5)
-Potential active food
packaging material [174]
Foods 2023,12, 2422 39 of 59
Table 3. Cont.
Packaging Material Characteristics of Food
Packaging System Mechanical Properties Thermal Properties Application Reference
Keratin–gelatin–
glycerin–curcumin
•Enhanced
mechanical
properties
•
Antibacterial activity
against S. aureus and
E. coli
TS(MPa): 12.45, 13.73
(respectively, for 7%
keratin–10% gelatin–1%
curcumin, 7% keratin–10%
gelatin–2% glycerin–1%
curcumin)
The initial
degradation weight
loss occurs between
25 ◦C and 130 ◦C
The second
degradation step is
observed in the
temperature range of
130–400 ◦C
The third step of
degradation occurs
between 400 and
800 ◦C
Potential active food
packaging material [175]
Whey proteins
Whey protein–
furcellaran–yerba
mate–white tea
extracts
•Improved water
vapor permeability,
water content,
solubility, tensile
strength, mechanical
properties, and
thermal stability
TS(MPa): 1.36 ±0.32,
1.31 ±0.20 (respectively,
for whey
protein–furcellaran, whey
protein—furcellaran–
yerba mate–white tea
extracts)
EB (%): 25.99 ±3.32,
25.13 ±2.79 (respectively,
for whey
protein–furcellaran, whey
protein–furcellaran–yerba
mate–white tea extracts)
Peak temperature
(Tm) (◦C) (1st
transition
endothermic):
218.2 ±1.1,
219.4 ±2.3
(respectively, for
whey
protein–furcellaran,
whey protein–
furcellaran–yerba
mate–white tea
extracts)
Potential edible film
for cheese packaging
with decreased
microbial growth and
water content
[52]
Whey protein-corn
oil—TiO2NPs
•Improved of
mechanical and
tensile properties
TS(MPa): 8.62 ±0.59,
16.24 ±0.29 (respectively,
for 2.5% whey
protein–corn oil–0% TiO2
NPs, 2.5% whey
protein–corn oil–0.5%
TiO2NPs)
EB (%): 30 ±8, 67 ±7
(respectively, for 2.5%
whey protein–corn oil–0%
TiO2NPs, 2.5% whey
protein–corn oil–0.5%
TiO2NPs)
The first stage of
weight loss 50 to
110 ◦C
The second stage of
weight loss
120–220 ◦C
The third stage of
weight loss
250–340 ◦C
Finally stage of
weight loss 350 to
500 ◦C
Potential active food
packaging material
for cheese packaging
[50]
Whey
protein–chitosan
nanofiber–nano-
formulated cinnamon
oil
•
Improved UV barrier
properties and
antibacterial activity
•Decrease in water
solubility and the
water vapor
permeability
•Slight reduction in
tensile strength
TS(MPa): 4.09 ±0.38,
3.41 ±0.47 (respectively,
for whey protein, whey
protein–chitosan
nanofiber–nano-
formulated cinnamon oil)
EB (%): 77.21 ±0.49,
35.57 ±5.85 (respectively,
for whey protein, whey
protein–chitosan
nanofiber–nano-
formulated
cinnamon oil)
Potential active food
packaging material [163]
Foods 2023,12, 2422 40 of 59
Table 3. Cont.
Packaging Material Characteristics of Food
Packaging System Mechanical Properties Thermal Properties Application Reference
Whey protein
isolate-coated
multilayer film
•Improved oxygen
and water vapor
permeability
TS(MPa): 45.80 ±1.53,
33.57 ±0.93 (respectively,
for polyethylene
terephthalate–whey
protein isolate,
low-density
polyethylene–linear
low-density polyethylene,
polyethylene
terephthalate–whey
protein isolate,
low-density
polyethylene–linear
low-density
polyethylene–aluminum
oxide)
EB (%): 84.10 ±14.67,
60.56 ±4.94 (respectively,
for polyethylene
terephthalate–whey
protein isolate,
low-density
polyethylene–linear
low-density polyethylene,
polyethylene
terephthalate–whey
protein isolate,
low-density
polyethylene–linear
low-density
polyethylene–aluminum
oxide)
Preservation of
physicochemical and
sensory properties of
frozen marinated
meatloaf up to
6 months
Potential frozen food
packaging material
[53]
Whey protein—
nanoemulsions of
orange peel (Citrus
sinensis) essential oil
•Improved water
barrier properties
and antioxidant and
antimicrobial
activities
TS(MPa): 2.64 ±0.62,
1.76 ±0.44 (respectively,
for whey protein, whey
protein—5% of
nanoemulsions of
Citrus sinensis)
EB (%): 11.40 ±1.68,
18.65 ±1.78 (respectively,
for whey protein, whey
protein—5% of
nanoemulsions of
Citrus sinensis)
-
Suitable active food
packaging material
for the preservation
of food against
oxidation and
microbial spoilage
[51]
Whey protein
isolate–polyvinyl
alcohol–nano-silica
•Improved water
barrier properties
and tensile strength
TS(MPa): 7.13, 10.2
(respectively, for whey
protein isolate–polyvinyl
alcohol, whey protein
isolate–polyvinyl
alcohol–4% nano silica)
Tg (◦C): 19, 26
(respectively, for
whey protein
isolate–polyvinyl
alcohol, whey protein
isolate–polyvinyl
alcohol–4% nano
silica)
Potential active food
packaging material [176]
Foods 2023,12, 2422 41 of 59
Table 3. Cont.
Packaging Material Characteristics of Food
Packaging System Mechanical Properties Thermal Properties Application Reference
Zein
Zein–potato
starch–chitosan NPs
incorporated with
curcumin
•Improved
mechanical and
barrier properties.
High oxidation
resistance and
relative release
efficiency
TS(MPa): 7.9 ±0.8,
13.1
±
2.3 (respectively, for
zein–potato starch,
zein–potato
starch–chitosan NPs
incorporated with
curcumin)
EB (%): 19.1 ±1.6,
50.3
±
4.1 (respectively, for
zein–potato starch,
zein–potato
starch–chitosan NPs
incorporated with
curcumin)
-
Delayed
physicochemical
changes in
Schizothorax prenati
fillets and prolonged
shelf-life up to
15 days. Potential
bioactive packaging
material for
Schizothorax prenati
fillets
[166]
Zein–chitosan–
cinnamodendron
dinisii schwanke
essential oil
•Improved
antioxidant activity
and antimicrobial
activity
-
The endothermic
peaks at −7.8 ◦C and
−6.2 ◦C (respectively,
for zein,
zein–chitosan–
Cinnamodendron
dinisii schwanke
essential oil)
Stabilizing
deterioration
reactions and
preserving the color
of ground beef
[55]
Zein-sodium
alginate-TiO2
NPs-betanin
•Improved
mechanical
properties, high
surface
hydrophobicity,
antioxidant and
antibacterial activity
•No in-vitro cell
cytotoxicity
TS(MPa): 2.01 ±0.26,
12.62 ±1.24 (respectively,
for zein–sodium alginate,
zein–sodium alginate-TiO
2
NPs–betanin)
EB (%): 10.74 ±2.11, 40.49
±3.72 (respectively, for
zein–sodium alginate,
zein–sodium alginate-TiO
2
NPs–betanin)
-Potential active food
packaging material [56]
Zein–pomegranate
peel extract–chitosan
NPs
•Improved thermal
stability and
antimicrobial activity
against L.
monocytogenes
TS(MPa): 12.22 ±1.2,
28 ±1.06 (respectively, for
zein, zein–pomegranate
peel extract–chitosan NPs)
EB (%): 2.6 ±0.22,
4.1
±
0.21 (respectively, for
zein, zein–pomegranate
peel extract–chitosan NPs)
The initial stage
happened between
100 and 150 ◦C.
The second stage of
weight loss occurred
at 200–250 ◦C
Restricted microbial
growth in pork
sample. Potential
antimicrobial active
food packaging
material
[167]
Zein-TiO2nanofibers
•Improved thermal
properties and
ethylene absorption
capability
•No significant
differences in water
contact angles
-
Zein nanofibers (0%
TiO2) presented a
one-step weight loss
which peaked at
approximately
240–390 ◦C
Potential active food
packaging material [54]
Zein–catechin-
loaded
β-cyclodextrin metal
•Decreased water
vapor permeability
and swelling degree
•Increased tensile
strength and
elongation at break
•Improved the
antioxidant activity
•Antimicrobial
activity against E.
coli and S. aureus
TS(MPa): 2.53 ±0.18,
19.24 ±0.61 (respectively,
for zein, zein–8%
catechin-loaded
β-cyclodextrin metal)
EB (%): 1.65 ±0.04,
4.51 ±0.14 (respectively,
for zein, zein–8%
catechin-loaded
β-cyclodextrin metal)
-Potential active food
packaging material [177]
Foods 2023,12, 2422 42 of 59
Table 3. Cont.
Packaging Material Characteristics of Food
Packaging System Mechanical Properties Thermal Properties Application Reference
Collagen
Collagen–chitosan–
lemon essential
oil
•Improved tensile
strength, elongation
at break and low
oxygen permeability
TS (MPa): 30.97 ±5.26,
20.73 ±3.88 (respectively,
for collagen,
collagen–chitosan–lemon
essential oil 40%)
EB (%): 65.41 ±10.28,
84.57
±
11.12 (respectively,
for collagen,
collagen–chitosan–lemon
essential oil 40%)
-
Delay deterioration
of pork at 4 ◦C for
21 days by
preventing lipid
oxidation and
microbial
proliferation
[60]
Collagen–alginate-
SiO2
•Reduction in
moisture content,
water vapor
transmission rate,
and water vapor
permeability
- - Potential active food
packaging material [169]
PLA shows incredible properties for films for food packaging applications such as
mechanical strength, light transmission, transparency, rigidity, low cost, high stiffness,
resilience, biodegradability, excellent barrier properties, and biocompatibility. However, it
is brittle, has low melt strength, and has low thermal stability [9,62,84,98].
In recent years, many different types of nanofillers have been incorporated into the
PLA matrix. Kostic et al. [
62
] incorporated alginate microbeads containing AgNPs into
a PLA matrix to form a nanocomposite film by using the solvent casting method. Here,
the PLA matrix acted as a diffusion barrier by lowering the Ag migration levels within
the allowed limit of 0.05 mg kg
−1
after 10 days. Further, the films had inhibitory effects
against S. aureus. While the incorporation of modified carbon nanostructures in the PLA
matrix increases the thermal and mechanical properties of the film [
84
]. On the other
hand, the studies of Andrade-Del Olmo et al. [
178
] focused on forming a layer-by-layer bio-
nanocomposite film of PLA-ZnONPs–chitosan-
β
-cyclodextrins. Here, PLA was blended
internally with ZnONPs, and it was superficially modified by the deposition of chitosan
and cyclodextrins. The microbial properties of treated surfaces were improved as a result
of increased surface hydrophilicity. The multilayers appear to be acceptable substrates for
carvacrol loading and release, with maximum release occurring during the first 14 days
of exposure.
Further, the incorporation of active agents’ thymol, kesum, and curry into a PLA
to form an active film through the solvent casting method was carried out in [
98
]. The
films showed antimicrobial activity against S. aureus. All active-agent-loaded PLA films
successfully kept chicken flesh in good condition during storage for up to 15 days. Yang
et al. [
67
] developed a packaging film by grafting star-like lignin microparticles onto PLA
via the ring open polymerization of l-lactide, which began with the hydroxyl groups on the
lignin microparticle surface. With the addition of lignin microparticles, elongation at break
increased up to 236%, and there was excellent UV resistance behavior, antioxidant activity,
and low migration level, making it a suitable packaging material.
6.3.2. Poly (Butylene Adipate Terephthalate) (PBAT)
Poly (butylene adipate terephthalate) (PBAT) is an aliphatic-aromatic copolyester
obtained from the poly-condensation of butanediol, adipic acid, and terephthalic acid [
95
].
It has been used for applications in agricultural, food packaging, and biomedical areas. The
major commercially available PBAT biopolymers are manufactured in BASF (ECOFLEX®,
Ludwigshafen, Germany), KINGFA (ECOPOND
®
, Guangzhou, China), NOVAMONT
(Origo-Bi
®
, Novara, Italy), TUNHE (Beijing, China), XINFU (Beijing, China), and JINHUI
Foods 2023,12, 2422 43 of 59
(ECOWORD
®
, Lvliang, China). Shopping bags have been developed using Starch-PBAT
blends by KINGFA, which is widely used in Chinese supermarkets [80].
PBAT has good mechanical and biodegradable properties. However, it has poor
photostability, which leads to a decline in its mechanical performance during the application.
Furthermore, it has high melt viscosity, low crystallization rate, low tensile strength, and
high production cost. Therefore, it is usually used in an application with blended polymers,
nanofillers, or other natural compounds [
9
,
66
,
179
]. Thus, blended products of starch-PBAT
and PLA-PBAT have been developed by KINGFA, China, to improve the mechanical
properties and production cost.
Recent studies have been performed with PBAT blended polymers. Sharma et al. [
64
]
developed a PLA-PBAT–ferulic acid, and this film was incorporated with ferulic acid by
using the solvent casting method. The thickness of the film was raised by 1.5–10%, and
tensile strength increased to 10.78 MPa from 5.42 MPa (control film) when ferulic acid was
added to the film. The film also showed antimicrobial activity against Listeria monocytogenes
and E. coli.
Further studies have been performed by incorporating lignin or melanin or lignin–
melanin core-shell into a PBAT matrix [
35
] as shown in Figure 8. At 0.5 to 5 wt% NP
concentrations, all of these films had outstanding UV-blocking capacity, blocking nearly all
UV-A and more than 80% of UV-B light while maintaining reasonable optical transparency.
4
Figure 8.
Development of Lignin nanoparticle and PBAT-based food packaging material.
Reprinted/adapted with permission from Ref. [35]. 2019, Elsevier.
6.3.3. Polycaprolactone (PCL)
Polycaprolactone (PCL) is a biodegradable polyester with a low melting point of 60
◦
C
and a glass transition temperature of
−
60
◦
C. It is prepared by the ring-opening polymer-
ization of
ε
-caprolactone. It has poor mechanical and thermal properties, high solubility,
and an excellent ability to form blends. Lukic, Vulic, and Ivanovic, [
180
] developed a blend
packaging material PCL-PLA–thymol–carvacrol by using the solvent casting method. The
thymol and carvacrol were loaded into the PCL-PLA mixture by utilizing supercritical CO
2
at 40
◦
C and 10 MPa for 5 h. The PCL-PLA film loaded with the thymol and carvacrol
mixture had the highest total polyphenol content (128.05 mg GAE/g film) and antioxidant
activity (7590.0
µ
molTrolox equivalent/g film), acceptable physical properties, and the
lowest release rate of 44.51 mg/L released after 6 weeks.
6.3.4. Polybutylene Succinate (PBS)
Polybutylene succinate (PBS) is a thermoplastic biodegradable aliphatic polyester
formed by polycondensation. It has properties similar to polypropylene with high crys-
tallinity and good thermal and mechanical properties. PBS has been used as an additive
with other biopolymers such as PLA [
67
]. A blended film of PBS-PLA was developed
Foods 2023,12, 2422 44 of 59
with the incorporation of carvacrol and thymol by the extrusion casting method [
180
]. The
inclusion of active compounds increased the ductility and flexibility of PLA-PBSA-based
active films. PLA-PBSA films with carvacrol or thymol had a high release of the active
compound and high antioxidant effectiveness. The spoilage and deterioration of salmon
slices were minimized, resulting in a 3–4-day extension of the shelf-life during cold storage.
6.3.5. Polyhydroxyalkanoate (PHAs)
Polyhydroxyalkanoate (PHAs) is a biodegradable, intracellular, and biocompatible
family of bacterial polyesters, which are produced by bacterial fermentation of sugar and
lipids. They have similar mechanical and thermal properties to synthetic polypropylene.
The merits of PHA include good tensile strength, printability, flavor and odor, barrier
properties, and temperature stability. The application of PHA is limited due to its high
cost. Different polymers of PHAs have been produced by different substrates; Poly-3-
(hydroxybutyrate-co-3-hydroxyvalerate) (PHBV) is produced from starch, vinnase, ethanol
stillage, and cheese whey, while Poly-3-(hydroxybutyrate) (PHB) is produced from molasses
wastewater and date syrup. Similarly, poly-
β
-hydroxyvalerate (PHV) is produced from
molasses wastewater. PHA is used for industrial applications such as in the pharmaceutical,
medical products, cosmetics, agriculture, aerospace, and food packaging industries. During
industrial applications, PHAs can be used as raw materials or as blends with other polymers
such as PLA, PBS, and PCL [
181
]. PHA is used as a biodegradable packaging application in
bottles, containers, sheets, films, laminates, fibers, and coatings manufacturing. Metabolix
(US) produces Metabolix PHA (blend of PHB and poly 3-hydroxyoctanoate) for food
packaging and additive application [170,182].
Table 4. Applications of aliphatic polyester biopolymers in food packaging.
Packaging Material Characteristics of Food
Packaging System Mechanical Properties Thermal Properties Application Reference
Poly lactic acid (PLA)
PLA-cellulose
nanocrystals–green
tea extract
•Improved barrier
properties,
antioxidant activity,
and effectiveness in
retarding lipid
oxidation
•Reduced oxygen
transmission ratio
and water vapor
permeability
TS(MPa): 39.8 ±5.8,
36.3
±
3.5 (respectively, for
PLA, PLA-2% cellulose
nanocrystals–green tea
extract)
EB (%): 2.7 ±0.4, 2.3 ±0.1
(respectively, for PLA,
PLA-2% cellulose
nanocrystals–green tea
extract)
Tg (◦C): 63.2, 59.6
(respectively, for PLA,
PLA-2% cellulose
nanocrystals–green
tea extract)
Extended the
shelf-life of salami
slices exhibiting an
oxidation reduction
[65]
PLA—alginate
microbeads
containing silver NPs
•Improved thermal
properties and
Young’s modulus
and reduced
elongation at break
•Antimicrobial
activity against
S. aureus
TS(MPa): 15.5 ±1.5,
14.0
±
1.1 (respectively, for
PLA, PLA composite)
EB (%): 477 ±26, 77 ±23
(respectively, for PLA,
PLA composite)
-Potential active food
packaging material [94]
PLA—carbon NPs
•Improved the
thermal and
mechanical
resistance
-
Tg (◦C): 280, 215
(respectively, for PLA,
PLA—0.09% carbon
nanotubes)
Potential active food
packaging material [183]
Foods 2023,12, 2422 45 of 59
Table 4. Cont.
Packaging Material Characteristics of Food
Packaging System Mechanical Properties Thermal Properties Application Reference
PLA—thymol–
kesum–curry
•Improved thermal
stability and water
vapor barrier
properties
•Antimicrobial
activity against
S. aureus and no
antimicrobial activity
against E. coli
-
Initial decomposition
temperature (◦C):
352.9, 342.7
(respectively, for PLA,
PLA—thymol–
kesum–curry)
Increased shelf-life of
chicken up to 15 days.
Active packaging
material suitable for
meats, fruits, and
vegetables products
[98]
PLA—lignin micro
particles
•
Improved elongation
at break, UV
resistance, and
antioxidant activity
-
Tg (◦C): 62.1 ±0.3,
64.8 ±0.4
(respectively, for PLA,
PLA—
ethylene−vinyl
acetate−glycidyl
methacrylate)
Potential active food
packaging material [184]
PLA—ZnO NPs
•Enhanced thermal
stability
•Antimicrobial
activity against
S. aureus and E. coli.
-
Tg (◦C): The pure
PLA film has shown
Tg around 60 ◦C and
Tm around 156 ◦C
Potential active food
packaging material [185]
PLA—fenugreek
essential
oil-curcumin
•
Improved UV barrier
properties, surface
color, tensile
strength, flexibility,
thickness, and water
contact angle
•Enhanced
antibacterial and
antioxidant
properties
TS(MPa): 30.27 ±1.0,
36.79 ±0.88 (respectively,
for PLA, PLA—fenugreek
essential oil–curcumin)
EB (%): 16.68 ±1.68, 53.08
±5.12 (respectively, for
PLA, PLA—fenugreek
essential oil–curcumin)
Tg (◦C): 58.67, 63.02
(respectively, for PLA,
PLA—fenugreek
essential
oil–curcumin)
Potential active food
packaging material [186]
PLA—PBAT-tannic
acid–gallic acid
•Enhance UV
blocking properties
and surface
hydrophobicity
•Antimicrobial
activity against
E. coli and
L. monocytogenes
TS(MPa): 4.80 ±0.06,
8.63 ±0.3, 7.01 ±0.95
(respectively, for PLA,
PLA-PBAT-10% tannic
acid, PLA,
PLA-PBAT—10% gallic
acid)
EB (%): 21.94 ±11.42,
23.52 ±9.18, 22.09 ±18.64
(respectively, for PLA,
PLA-PBAT—10% tannic
acid, PLA,
PLA-PBAT—10%
gallic acid)
The first weight loss
at around 30 to 70 ◦C
Potential active food
packaging material [187]
Poly(butylene adipate terephthalate) (PBAT)
PBAT-PLA—ferulic
acid
•Improved tensile
strength and UV
light barrier
properties
•
Antibacterial activity
against
L. monocytogenes and
E. coli
TS(MPa): 5.42 ±0.03,
10.78 ±0.83 (respectively,
for PBAT-PLA,
PBAT-PLA—ferulic acid)
EB (%): 21.93 ±17.42,
22.13
±
21.34 (respectively,
for PBAT-PLA,
PBAT-PLA—ferulic acid)
The first weight loss
stage was around 60
to 80 ◦C
Potential active food
packaging material [64]
Foods 2023,12, 2422 46 of 59
Table 4. Cont.
Packaging Material Characteristics of Food
Packaging System Mechanical Properties Thermal Properties Application Reference
PBAT-lignin—
melanin
NPs
•
Improved UV barrier
capability,
photostability, tensile
properties, and
thermal stability
One-step
degradation process
with an
initial decomposition
temperature of
369 ◦C
major
weight loss occurring
around 400 ◦C
Potential active food
packaging material
where high UV
resistance is required
[35]
PBAT-PLA—nano-
polyhedral
oligomeric
silsesquioxane
•Improved
mechanical
properties, water
vapor, CO2and O2
permeability
- - Potential active food
packaging material [9]
PBAT—glycerol–
zeolite–citric
acid–cassava starch
•Improved
mechanical
properties and Water
vapor permeability
TS(MPa): 2.44 ±0.23,
2.44 ±0.24 (respectively,
for control films, zeolites)
EB (%): 74.84 ±23.74,
97.74
±
19.99 (respectively,
for control films, zeolites)
Preserved the color
and vitamin C
content broccoli
florets for 7 days.
Senescence indicator
of labels were able to
detect CO2
in packages
[188]
PBAT-PLA—
carvacrol
•
Reduced permeation
of vapor and oxygen
•Delayed fungal
growth and
sporulation of
Penicillium sp. and
Rhizopus sp.
•Increased shelf-life
of packaged bread
and butter cake by
2.0–2.3 times
TS(MPa): 26.8 ±3.9,
16.4
±
1.4 (respectively, for
PBAT 70-PLA 30, PBAT
70-PLA 30—5% carvacrol)
EB (%): 267.3 ±37.3
(respectively, for PBAT
70-PLA 30, PBAT 70-PLA
30—5% carvacrol)
Weight loss at
degradation
temperatures of 100,
310 and 350 ◦C
Potential active food
packaging material [189]
PBAT—zinc
oxide–graphene
oxide
•Improved the
mechanical and
thermal properties
•
Antibacterial activity
against E.coli
(81.32%) and
S. aureus (82.44%)
TS(MPa): 7.65 ±0.55,
27.43 ±0.83 (respectively,
for PBAT, PBAT—zinc
oxide–graphene oxide)
EB (%): 121.96 ±6.35,
304.38 ±14.84
(respectively, for PBAT,
PBAT—zinc
oxide–graphene oxide)
Final thermal
decomposition at
about 650 ◦C
Potential active food
packaging material [190]
PBAT—SiO2
NP-grape seed
essential oil
•Improved
antimicrobial
activities, film
flexibility, and
optical and heat
resistance properties
TS(MPa): 35, 43
(respectively, for PBAT,
PBAT-GEO-SiO2NP
(87:10:3))
EB (%): 590, 595
(respectively, for PBAT,
PBAT-GEO-SiO2NP
(87:10:3))
Initial weight loss at
temperatures of
70–90 ◦C.
Second thermal
decomposition at
320–411 ◦C
Potential active food
packaging material [179]
Poly caprolactone (PCL)
PCL-PLA—thymol–
carvacrol
•High total
polyphenol content,
increased
antioxidant activity,
good storage
stability, acceptable
physical properties,
and low release rate
TS(MPa): 29.6 ±1.47,
6.42
±
0.6783 (respectively,
for PCL–PLA, PCL-PLA—
thymol–carvacrolzinc
oxide–graphene oxide)
EB (%): 603.4 ±48.7, 10.68
±2.30 (respectively, for
PCL –PLA, PCL-PLA-
thymol–carvacrolzinc
oxide–graphene oxide)
-Potential active food
packaging material [180]
Foods 2023,12, 2422 47 of 59
Table 4. Cont.
Packaging Material Characteristics of Food
Packaging System Mechanical Properties Thermal Properties Application Reference
PCL-α-tocopherol
•High antioxidant
activity
•Reduction of
microbial growth on
cheese
- - Potential active food
packaging material [191]
PCL-poly(propylene
carbonate)
•
Improved gas barrier
property and water
vapor permeability
•Extended the
shelf-life of button
mushroom up to 17
days of storage.
TS(MPa): 9.6 ±1.0,
19.9
±
0.9 (respectively, for
PCL-40, PCL-60)
EB (%): 371 ±43.9,
465 ±36.9 (respectively,
for PCL-40, PCL-60)
-Potential active food
packaging material [192]
Poly (butylene succinate adipate) (PBSA)
PBSA-PLA
•Improved
mechanical,
antibacterial, and
antioxidant
properties
TS(MPa): 48.61 ±1.22,
36.68 ±1.74 (respectively,
for 90 wt% PLA +10 wt%
PBSA, 82.8 wt% PLA +9.2
wt% PBSA +8 wt%
Thymol)
EB (%): 55.70 ±3.56,
353.80 ±24.80b
(respectively, for 90 wt%
PLA +10 wt% PBSA, 82.8
wt% PLA +9.2 wt% PBSA
+8 wt% Thymol)
Endothermic peak of
melting at 149 ◦C
Extended the
shelf-life of salmon
slices by 3–4 days
during cold storage.
Active packaging
material suitable for
fishery products
[67]
PBSA-poly(3-
hydroxybutyrate-co-
3-hydroxyvalerate)
•Improved melt
viscosity and
accelerated
crystallization
kinetics
TS(MPa): 2153, 1297
(respectively, for
PHBV/PBSA 100/0,
PHBV/PBSA 70/30)
EB (%): 0.98 ±0.1,
134.8 ±48 (respectively,
for PHBV/PBSA 100/0,
PHBV/PBSA 70/30)
Tm (◦C): 88 ±3,
86 ±2, (respectively,
for PHBV/PBSA
0/100, PHBV/PBSA
70/30)
Tg (◦C): −45.9 ±1.6,
−48.6 ±2.3
(respectively, for
PHBV/PBSA 0/100,
PHBV/PBSA 70/30)
Potential active food
packaging material [193]
Polyhydroxyalkanoate (PHAs)
PHB-graphene
nanoplatelets
•Improved thermal
stability, barrier
properties, and
tensile strength
•Decreased oxygen
and water vapor
permeability
•Statistically
insignificant
cytotoxic effect
TS (MPa): 4.5, 12.2
(respectively, for PHB,
PHB-1.3 wt% graphene
nanoplatelets)
Tmax: 279.4 ◦C,
284.1
◦
C (respectively,
for PHB, PHB-1.3
wt% graphene
nanoplatelets)
Active packaging
material suitable for
moisture and
oxygen-sensitive
food items (potato
chips and milk
product)
[190]
PHB-
polycaprolactone-
organo-clays
(Cloisite®30 B and
10A)
•Improved barrier
properties and
degradation
temperature
•Antimicrobial
activity against
Lactobacillus
plantarum
TS(MPa): 6.29 ±1.42,
7.06 ±1.96 (respectively,
for PHB-PLA,
PHB-PLA-Cloisite®30 B)
EB (%): 3.03 ±1.71,
0.72 ±0.19 (respectively,
for PHB-PLA,
PHB-PLA-Cloisite®30 B)
Increased shelf-life of
sliced ham. Active
packaging material
suitable for processed
meat packaging
[69]
Foods 2023,12, 2422 48 of 59
Table 4. Cont.
Packaging Material Characteristics of Food
Packaging System Mechanical Properties Thermal Properties Application Reference
PHBV-PHB-eugenol
•Improved
hydrophobicity,
mechanical, and
thermal barrier
properties.
•Strong adhesion and
high electro
spinnability
•Antimicrobial
activity against
S. aureus and E. coli
TS(MPa): 1491 ±207,
1446 ±190 (respectively,
for active multilayer with
cellulose nanocrystal,
active multilayer with
cellulose nanocrystal)
EB (%): 59.1 ±56,
51.6 ±45 (respectively, for
active multilayer with
cellulose nanocrystal,
active multilayer with
cellulose nanocrystal)
-
Potential multilayer
antimicrobial active
food packaging
material
[70]
PHBV-PHB–cellulose
nanofibrils-
lignocellulose
nanofibrils
•Improved water
contact resistance,
mechanical and
water vapor and
oxygen barrier
properties
•
Slightly lower aroma
barrier properties
TS(MPa): 4504.2 ±105,
2991.4 ±184 (respectively,
for cellulose nanofibrils,
lignocellulose nanofibrils)
EB (%): 18.1 ±2.2,
13.7
±
0.5 (respectively, for
cellulose nanofibrils,
lignocellulose nanofibrils)
-Potential active food
packaging material [194]
PHBV-thermoplastic
starch
•Improved oxygen
barrier properties,
reduce water uptake
•Oxygen barrier
properties are
slightly
compromised
- -
Build on current
knowledge on
multilayered
TPS-PHBV film for
food packaging
applications
[195]
PHA-cellulose
nanocrystals
•Good interlayer
adhesion and contact
transparency
•Enhanced
mechanical
properties
TS(MPa): 24.5 ±0.6,
39.0
±
1.9 (respectively, for
poly(3-hydroxybutyrate-
co-3-hydroxyvalerate)
(PHBV) containing
8 mol.%, 2 mol.%
EB (%): 2.6 ±0.2, 1.4 ±0.1
(respectively, for
poly(3-hydroxybutyrate-
co-3-hydroxyvalerate)
(PHBV) containing 8
mol.%, 2 mol.%
-Potential active food
packaging material [182]
Polyhydroxybutyrate (PHB) is the most abundant PHAs that is a biodegradable lipid-
like polymer synthesized by different bacteria that has a rigid structure. It is suitable as a
food packaging material since it is renewable, biocompatible, and has low oxygen and water
permeability and increased barrier properties. A study by Rech et al. [
193
] combined PHB
with essential oils (cinnamon, melaleuca, and citronella) to form an edible film for food pack-
aging by using the solution casting method. Essential oils increased both the crystallinity
degree and the thermal stability of PHB films. Furthermore, by lowering the melting
temperature from 155.7
◦
C to 143.7
◦
C (melaleuca-cinnamon) and increasing film flexibility
by the reduction in the elastic modulus from 1030 MPa to 286 MPa (melaleuca-cinnamon) of
the polymer, these oils created a plasticizing effect. Additional studies on PHB incorporated
with NPs were performed by PHB-graphene nanoplatelets [
69
] and PHB-polycaprolactone
(PCL)-organo-clays [
70
]. Manikandan et al. [
69
] formed a PHB nanocomposite film by
incorporating different concentrations of graphene nanoplatelets (0–1.3 wt%) via the so-
lution casting method. The incorporation of graphene nanoplatelets into PHB increased
the melting point by 10
◦
C, thermal stability (by 10
◦
C), tensile strength by 2 times, and
reduced oxygen and water vapor permeability by 3 and 2 times, respectively. Further,
Foods 2023,12, 2422 49 of 59
there was a four-fold increase in the shelf-life of potato chips and milk products. Correa
et al. [
70
]] incorporated organo-clays (Cloisite
®
30 B and 10A) into a matrix of PHB/PCL
by melt intercalation, and the nanocomposite films were formed by compression molding.
Although organo-clays have antimicrobial activity against Lactiplantibacillus plantarum, their
incorporation in the polymer blend did not result in antimicrobial films. However, the nisin-
activated PHB-PCL film showed antimicrobial activity against Lactiplantibacillus plantarum
by prolonging the shelf-life of sliced ham. Poly(3-hydroxybutyrate-co-3-hydroxyvalerate)
(PHBV) has higher processability and physical properties than PHB. PHBV also has high
flexibility, toughness, and low melting point. Recently, Figueroa-Lopez et al. [
170
] devel-
oped a multilayer PHBV-PHB-eugenol active food packaging material by incorporating
different concentrations of eugenol into the PHBV ultra-thin fibers by electrospinning.
Then, this PHBV monolayer was interlaid between PHB sheets by annealing at 160
◦
C for
10 s to form a multilayer active packaging material. This film showed high hydrophobicity
of 75.53 and improved mechanical (tensile strength improved from 1252 MPa to 2884 MPa
with the addition of 2.5 wt.% of eugenol to PHBV), thermal, barrier, and antimicrobial
(against S. aureus and E. coli) properties. Further studies were performed on developing
PHBV-PHB–cellulose nanofibrils–lignocellulose nanofibrils containing mono- and multi-
layer films by using the electrospinning coating technique [
170
]. The multilayer film with
PHBV-PHB–cellulose nanofibrils–lignocellulose nanofibrils reduced oxygen permeance by
35% when compared to the control film, thus having enhanced gas barrier performance.
7. SWOT Analysis of Biodegradable Polymers in the Food Packaging Industry
7.1. Strengths
Biopolymers are eco-friendly, biodegradable, nontoxic, renewable, and biocompatible
alternatives to synthetic packaging materials. These are easily recycled, avoiding the
environmental pollution caused by synthetic polymers while addressing the important
question of environmental pollution. Thus, it is environmentally friendly and possesses a
much lower risk than synthetic products. Biopolymers are naturally occurring in animals,
plants, and microorganisms and are thus highly abundant. The extraction process and the
synthesis depend on the different biopolymers.
They have great film-forming ability and different strengths specific to each biopoly-
mer as discussed above. Biopolymers can create high-performance packaging materials
together with other biopolymers or reinforcement agents, and they are lightweight. Biopoly-
mers work as matrices to incorporate nanofillers, natural compounds, antimicrobial agents,
antioxidants, vitamins, minerals, and nutrients to make them more suitable active packag-
ing materials.
7.2. Weaknesses
Even though biopolymers are environmentally friendly, their main weaknesses are low
mechanical and barrier properties, rapid degradation rate, high hydrophilic capacity, and
high sensitivity to moisture. In addition to the poor material performance, they also have
weak mechanical and chemical structures, making many of the biopolymers not suitable for
food packaging directly. Further, when compared to synthetic polymers, they are difficult
to process and relatively expensive. Most of the biopolymers are naturally hydrophilic
and deteriorate when exposed to moisture. The above-mentioned characteristics of the
biopolymers make them unsuitable as packaging materials since it makes them unsuitable
to maintain the shelf-life and quality of food products.
7.3. Opportunities
There are a wide variety of opportunities for using biopolymers in food packaging,
including active and smart food packaging materials. Biopolymers are the base compound
for most of the packaging material combinations along with nanomaterials or other active
compounds. The addition of the reinforcement agents into the biopolymer matrix results
in the improvement of essential properties needed in packaging material, such as barrier,
Foods 2023,12, 2422 50 of 59
mechanical, thermal, antioxidant, and antimicrobial properties. Most of the food packaging
materials developed are still in the research stage, and there is an opportunity for the
upscale and global production of these materials to use as an alternative to synthetic
polymers. Biopolymers and bioplastic industrial production possess the opportunity to
reduce global environmental pollution and aid the circular economy as mentioned by the
European Union.
7.4. Threats
While environmental concerns regarding plastic packaging are well-documented,
the assessment of biopolymers’ environmental impact is more nuanced. Biopolymers
have the potential to be more environmentally friendly, but their specific advantages and
disadvantages hinge on a number of variables, such as their origin, production processes,
waste management systems, and end-of-life considerations. To make informed decisions
about a material’s environmental impact, it is essential to conduct a thorough analysis of
the material’s life cycle. Most of the biopolymers in their pure form do not deliver a threat
to society or the environment. However, these biopolymers are combined with nanofillers
or other active agents to improve the qualities of the packaging materials. These agents
pose a threat of migration into a food product and gradually migrate into the human body.
This may cause a threat to human health if the agent is cytotoxic. Further, during the
biodegradation process, the active agents are migrated into soil/water, which may affect
environmental conditions, leading to pollution. The migration of chemical compounds
is not unique to biopolymers; it can also occur with other packaging materials. It is
essential to assess and manage the potential migration of compounds from any packaging
material, including biopolymers, to ensure food safety and regulatory compliance. Ongoing
research and development is aimed at enhancing the safety and efficacy of biopolymers
for food packaging applications. This includes the development of novel materials, the
optimization of processing techniques, and extensive testing to ensure their suitability
for food contact and to minimize the migration of potentially hazardous substances. In
addition, the microorganisms used to produce biopolymers may be hazardous and may
result in environmental pollution.
8. Future Trends and Conclusions
Over the years, synthetic packaging materials have been the primary source of food
packaging. However, the use of synthetic polymers presents challenges and limitations,
mainly due to environmental pollution issues caused by plastics. Consequently, the trend
of using biopolymers in food packaging has significantly increased in recent years. Biopoly-
mers/bioplastics such as thermoplastic starch, PLA, cellulose, and PBAT are already used
in industrial production for food packaging applications. Their characteristics, such as
biodegradability, eco-friendliness, renewability, nontoxicity, and lightweight properties,
make them suitable for food packaging applications. However, the applications of biopoly-
mers in their pure form are limited due to their low mechanical, barrier, and thermal
properties. Furthermore, they are less cost-effective compared to synthetic polymers. The
negative characteristics of biopolymers can be overcome by adding reinforcement agents
such as nanofillers and active agents. These reinforcing agents enhance the properties of the
packaging materials, making them suitable for active and intelligent packaging materials
by extending their shelf-life and enhancing the quality of packaged food products. In recent
years, researchers have focused on conducting studies on the combinations of biopolymers,
reinforcement agents, and their applications. However, there are limited studies carried
out using some biopolymers; for instance, the natural UV barrier property of lignin has
been studied in limited research. Moreover, when compared to starch-based biopolymers,
studies on protein biopolymers and some aliphatic biopolymers (PBS, PCL) are limited. The
food packaging applications of the produced biopolymers have only become an interest to
scientists in recent years, and there is still considerable room for improvement in research.
Furthermore, only a few studies have been performed to evaluate the cytotoxicity effect of
Foods 2023,12, 2422 51 of 59
the produced packaging material and the biodegradation ability of the materials. These
two aspects of the study are crucial to avoid global issues in the future. Additional studies
are warranted to bring biopolymer-based food packaging to a global level and use it as an
alternative to plastic packaging.
Author Contributions:
Conceptualization, S.J. and A.K.J.; writing—original draft preparation, K.Y.P.
writing—review and editing, K.Y.P., S.J. and A.K.J.; supervision, S.J. and A.K.J. All authors have read
and agreed to the published version of the manuscript.
Funding:
The present work was supported by Technological University Dublin-City Campus, Ireland,
under the TU Dublin Researcher Award 2021.
Data Availability Statement:
The data used to support the findings of this study can be made
available by the corresponding author upon request.
Conflicts of Interest: The authors declare no conflict of interest.
References
1.
Horst, C.; Pagno, C.H.; Flores, S.H.; Costa, T.M.H. Hybrid starch/silica films with improved mechanical properties. J. Sol-Gel Sci.
Technol. 2020,95, 52–65. [CrossRef]
2.
Chaudhary, P.; Fatima, F.; Kumar, A. Relevance of Nanomaterials in Food Packaging and Its Advanced Future Prospects. J. Inorg.
Organomet. Polym. Mater. 2020,30, 5180–5192. [CrossRef] [PubMed]
3.
Hou, X.; Xue, Z.; Xia, Y.; Qin, Y.; Zhang, G.; Liu, H.; Li, K. Effect of SiO
2
nanoparticle on the physical and chemical properties of
eco-friendly agar/sodium alginate nanocomposite film. Int. J. Biol. Macromol. 2019,125, 1289–1298. [CrossRef] [PubMed]
4.
Mostafavi, F.S.; Zaeim, D. Agar-based edible films for food packaging applications—A review. Int. J. Biol. Macromol.
2020
,159,
1165–1176. [CrossRef]
5.
Matthews, C.; Moran, F.; Jaiswal, A.K. A review on European Union’s strategy for plastics in a circular economy and its impact
on food safety. J. Clean. Prod. 2021,283, 125263. [CrossRef]
6.
Arezoo, E.; Mohammadreza, E.; Maryam, M.; Abdorreza, M.N. The synergistic effects of cinnamon essential oil and nano TiO
2
on
antimicrobial and functional properties of sago starch films. Int. J. Biol. Macromol. 2020,157, 743–751. [CrossRef]
7. Coelho, C.C.S.; Silva, R.B.S.; Carvalho, C.W.P.; Rossi, A.L.; Teixeira, J.A.; Freitas-Silva, O.; Cabral, L.M.C. Cellulose nanocrystals
from grape pomace and their use for the development of starch-based nanocomposite films. Int. J. Biol. Macromol.
2020
,159,
1048–1061. [CrossRef]
8.
Estevez-Areco, S.; Guz, L.; Candal, R.; Goyanes, S. Active bilayer films based on cassava starch incorporating ZnO nanorods and
PVA electrospun mats containing rosemary extract. Food Hydrocoll. 2020,108, 106054. [CrossRef]
9.
Zhai, X.; Wang, W.; Zhang, H.; Dai, Y.; Dong, H.; Hou, H. Effects of high starch content on the physicochemical properties of
starch/PBAT nanocomposite films prepared by extrusion blowing. Carbohydr. Polym. 2020,239, 116231. [CrossRef]
10.
Jha, P. Effect of plasticizer and antimicrobial agents on functional properties of bionanocomposite films based on corn starch-
chitosan for food packaging applications. Int. J. Biol. Macromol. 2020,160, 571–582. [CrossRef]
11.
Siripatrawan, U.; Kaewklin, P. Fabrication and characterization of chitosan-titanium dioxide nanocomposite film as ethylene
scavenging and antimicrobial active food packaging. Food Hydrocoll. 2018,84, 125–134. [CrossRef]
12.
Paiva, C.A.; Vilvert, J.C.; Menezes, F.L.G.; Leite, R.H.d.L.; Santos, F.K.G.; Medeiros, J.F.; Aroucha, E.M.M. Extended shelf life of
melons using chitosan and graphene oxide-based biodegradable bags. J. Food Process. Preserv. 2020,44, e14871. [CrossRef]
13.
de Lima Barizão, C.; Crepaldi, M.I.; Junior, O.D.O.S.; de Oliveira, A.C.; Martins, A.F.; Garcia, P.S.; Bonafé, E.G. Biodegradable
films based on commercial
κ
-carrageenan and cassava starch to achieve low production costs. Int. J. Biol. Macromol.
2020
,165,
582–590. [CrossRef] [PubMed]
14.
Yadav, M.; Liu, Y.-K.; Chiu, F.-C. Fabrication of Cellulose Nanocrystal/Silver/Alginate Bionanocomposite Films with Enhanced
Mechanical and Barrier Properties for Food Packaging Application. Nanomaterials 2019,9, 1523. [CrossRef] [PubMed]
15.
Al-Tayyar, N.A.; Youssef, A.M.; Al-hindi, R. Antimicrobial food packaging based on sustainable Bio-based materials for reducing
foodborne Pathogens: A review. Food Chem. 2020,310, 125915. [CrossRef]
16.
Nouri, A.; Tavakkoli Yaraki, M.; Lajevardi, A.; Rahimi, T.; Tanzifi, M.; Ghorbanpour, M. An investigation of the role of fabrication
process in the physicochemical properties of
κ
-carrageenan-based films incorporated with Zataria multiflora extract and nanoclay.
Food Packag. Shelf Life 2020,23, 100435. [CrossRef]
17.
Cazón, P.; Vázquez, M. Bacterial cellulose as a biodegradable food packaging material: A review. Food Hydrocoll.
2021
,113, 106530.
[CrossRef]
18.
Noshirvani, N.; Ghanbarzadeh, B.; Rezaei Mokarram, R.; Hashemi, M. Novel active packaging based on carboxymethyl cellulose-
chitosan-ZnO NPs nanocomposite for increasing the shelf life of bread. Food Packag. Shelf Life 2017,11, 106–114. [CrossRef]
19.
El-Hefnawy, M.E. Biodegradable Films from Phytosynthesized TiO
2
Nanoparticles and Nanofungal Chitosan as Probable
Nanofertilizers. Int. J. Polym. Sci. 2020,2020, 6727132. [CrossRef]
Foods 2023,12, 2422 52 of 59
20.
Salama, H.E.; Aziz, M.S.A. Optimized carboxymethyl cellulose and guanidinylated chitosan enriched with titanium oxide
nanoparticles of improved UV-barrier properties for the active packaging of green bell pepper. Int. J. Biol. Macromol.
2020
,165,
1187–1197. [CrossRef]
21.
Roy, S.; Rhim, J.-W. Agar-based antioxidant composite films incorporated with melanin nanoparticles. Food Hydrocoll.
2019
,94,
391–398. [CrossRef]
22.
Fekete, E.; Bella, E.; Csiszar, E.; Moczo, J. Improving physical properties and retrogradation of thermoplastic starch by incorporat-
ing agar. Int. J. Biol. Macromol. 2019,136, 1026–1033. [CrossRef]
23.
Jridi, M.; Abdelhedi, O.; Zouari, N.; Fakhfakh, N.; Nasri, M. Development and characterization of grey triggerfish gelatin/agar
bilayer and blend films containing vine leaves bioactive compounds. Food Hydrocoll. 2019,89, 370–378. [CrossRef]
24.
Gorrasi, G.; Bugatti, V.; Viscusi, G.; Vittoria, V. Physical and Barrier Properties of Chemically Modified Pectin with Polycaprolac-
tone through an Environmentally Friendly Process. Colloid Polym. Sci. 2021,299, 429–437. [CrossRef]
25.
Mellinas, A.C.; Jimenez, A.; Garrigos, M.C. Pectin-Based Films with Cocoa Bean Shell Waste Extract and ZnO/Zn-NPs with
Enhanced Oxygen Barrier, Ultraviolet Screen and Photocatalytic Properties. Foods 2020,9, 1572. [CrossRef] [PubMed]
26.
Gouveia, T.I.A.; Biernacki, K.; Castro, M.C.R.; Gonçalves, M.P.; Souza, H.K.S. A new approach to develop biodegradable films
based on thermoplastic pectin. Food Hydrocoll. 2019,97, 105175. [CrossRef]
27.
Norcino, L.B.; Mendes, J.F.; Natarelli, C.V.L.; Manrich, A.; Oliveira, J.E.; Mattoso, L.H.C. Pectin films loaded with copaiba oil
nanoemulsions for potential use as bio-based active packaging. Food Hydrocoll. 2020,106, 105862. [CrossRef]
28.
Cheikh, D.; Martín-Sampedro, R.; Majdoub, H.; Darder, M. Alginate Bionanocomposite Films Containing Sepiolite Modified with
Polyphenols from Myrtle Berries Extract. Int. J. Biol. Macromol. 2020,165, 2079–2088. [CrossRef]
29.
Perera, K.Y.; Sharma, S.; Duffy, B.; Pathania, S.; Jaiswal, A.K.; Jaiswal, S. An Active Biodegradable Layer-by-Layer Film Based on
Chitosan-Alginate-TiO2for the Enhanced Shelf Life of Tomatoes. Food Packag. Shelf Life 2022,34, 100971. [CrossRef]
30.
Cazón, P.; Velazquez, G.; Ramírez, J.A.; Vázquez, M. Polysaccharide-based films and coatings for food packaging: A review. Food
Hydrocoll. 2017,68, 136–148. [CrossRef]
31.
Ruan, C.; Zhang, Y.; Wang, J.; Sun, Y.; Gao, X.; Xiong, G.; Liang, J. Preparation and Antioxidant Activity of Sodium Alginate and
Carboxymethyl Cellulose Edible Films with Epigallocatechin Gallate. Int. J. Biol. Macromol. 2019,134, 1038–1044. [CrossRef]
32.
Pavli, F.; Argyri, A.A.; Skandamis, P.; Nychas, G.J.; Tassou, C.; Chorianopoulos, N. Antimicrobial Activity of Oregano Essential
Oil Incorporated in Sodium Alginate Edible Films: Control of Listeria monocytogenes and Spoilage in Ham Slices Treated with
High Pressure Processing. Materials 2019,12, 3726. [CrossRef] [PubMed]
33.
Raschip, I.E.; Fifere, N.; Varganici, C.D.; Dinu, M.V. Development of Antioxidant and Antimicrobial Xanthan-Based Cryogels
with Tuned Porous Morphology and Controlled Swelling Features. Int. J. Biol. Macromol. 2020,156, 608–620. [CrossRef]
34.
Rukmanikrishnan, B.; Ismail, F.R.M.; Manoharan, R.K.; Kim, S.S.; Lee, J. Blends of Gellan Gum/Xanthan Gum/Zinc Oxide Based
Nanocomposites for Packaging Application: Rheological and Antimicrobial Properties. Int. J. Biol. Macromol.
2020
,148, 1182–1189.
[CrossRef] [PubMed]
35.
Xing, Q.; Buono, P.; Ruch, D.; Dubois, P.; Wu, L.; Wang, W.J. Biodegradable UV-Blocking Films through Core-Shell Lignin-Melanin
Nanoparticles in Poly(Butylene Adipate-Co-Terephthalate). ACS Sustain. Chem. Eng. 2019,7, 4147–4157. [CrossRef]
36.
Zadeh, E.M.; O’Keefe, S.F.; Kim, Y.T. Utilization of Lignin in Biopolymeric Packaging Films. ACS Omega
2018
,3, 7388–7398.
[CrossRef]
37.
Dou, J.; Vuorinen, T.; Koivula, H.; Forsman, N.; Sipponen, M.; Hietala, S. Self-Standing Lignin-Containing Willow Bark
Nanocellulose Films for Oxygen Blocking and UV Shielding. ACS Appl. Nano Mater. 2021,4, 2921–2929. [CrossRef]
38.
Esakkimuthu, E.S.; DeVallance, D.; Pylypchuk, I.; Moreno, A.; Sipponen, M.H. Multifunctional lignin-poly (lactic acid) biocom-
posites for packaging applications. Bioeng. Biotechnol. 2022,10, 1025076. [CrossRef]
39.
Yeasmin, S.; Yeum, J.H.; Yang, S.B. Fabrication and characterization of pullulan-based nanocomposites reinforced with montmo-
rillonite and tempo cellulose nanofibril. Carbohydr. Polym. 2020,240, 116307. [CrossRef]
40.
Priyadarshi, R.; Kim, S.M.; Rhim, J.W. Pectin/pullulan blend films for food packaging: Effect of blending ratio. Food Chem.
2021
,
347, 129022. [CrossRef]
41.
Zhang, Y.; Zhou, L.; Zhang, C.; Show, P.L.; Du, A.; Fu, J.; Ashokkumar, V. Preparation and characterization of curdlan/polyvinyl
alcohol/ thyme essential oil blending film and its application to chilled meat preservation. Carbohydr. Polym.
2020
,247, 116670.
[CrossRef] [PubMed]
42.
Zhou, L.; Fu, J.; Bian, L.; Chang, T.; Zhang, C. Preparation of a novel curdlan/bacterial cellulose/cinnamon essential oil blending
film for food packaging application. Int. J. Biol. Macromol. 2022,212, 211–219. [CrossRef]
43.
Nilsuwan, K.; Guerrero, P.; Caba, K.D.L.; Benjakul, S.; Prodpran, T. Fish gelatin films laminated with emulsified gelatin film
or poly(lactic) acid film: Properties and their use as bags for storage of fried salmon skin. Food Hydrocoll.
2021
,111, 106199.
[CrossRef]
44.
Riahi, Z.; Priyadarshi, R.; Rhim, J.W.; Bagheri, R. Gelatin-based functional films integrated with grapefruit seed extract and TiO
2
for active food packaging applications. Food Hydrocoll. 2021,112, 106314. [CrossRef]
45.
Pattarasiriroj, K.; Kaewprachu, P.; Rawdkuen, S. Properties of rice flour-gelatine-nanoclay film with catechin-lysozyme and its
use for pork belly wrapping. Food Hydrocoll. 2020,107, 105951. [CrossRef]
46.
Zubair, M.; Ullah, A. Recent advances in protein derived bionanocomposites for food packaging applications. Crit. Rev. Food Sci.
Nutr. 2020,60, 406–434. [CrossRef]
Foods 2023,12, 2422 53 of 59
47.
Salarbashi, D.; Bazeli, J.; Tafaghodi, M. Environment-friendly green composites based on soluble soybean polysaccharide: A
review. Int. J. Biol. Macromol. 2019,122, 216–223. [CrossRef]
48.
Salarbashi, D.; Tafaghodi, M.; Bazzaz, B.S.F.; Birjand, S.M.A.; Bazeli, J. Characterization of a green nanocomposite prepared from
soluble soy bean polysaccharide/Cloisite 30B and evaluation of its toxicity. Int. J. Biol. Macromol. 2018,120, 109–118. [CrossRef]
49.
Salarbashi, D.; Tafaghodi, M.; Bazzaz, B.S.F.; Mohammad Aboutorabzade, S.; Fathi, M. pH-sensitive soluble soybean polysaccha-
ride/SiO2 incorporated with curcumin for intelligent packaging applications. Food Sci. Nutr. 2021,9, 2169–2179. [CrossRef]
50.
Montes-de-Oca-Ávalos, J.M.; Altamura, D.; Herrera, M.L.; Huck-Iriart, C.; Scattarella, F.; Siliqi, D.; Giannini, C.; Candal, R.J.
Physical and structural properties of whey protein concentrate—Corn oil—TiO2 nanocomposite films for edible food-packaging.
Food Packag. Shelf Life 2020,26, 100590. [CrossRef]
51.
Amjadi, S.; Almasi, H.; Ghadertaj, A.; Mehryar, L. Whey protein isolate-based films incorporated with nanoemulsions of orange
peel (Citrus sinensis) essential oil: Preparation and characterization. Food Process. Preserv. 2021,45, e15196. [CrossRef]
52.
Pluta-Kubica, A.; Jamróz, E.; Kawecka, A.; Juszczak, L.; Krzy´sciak, P. Active edible furcellaran/whey protein films with yerba
mate and white tea extracts: Preparation, characterization and its application to fresh soft rennet-curd cheese. Int. J. Biol. Macromol.
2020,155, 1307–1316. [CrossRef] [PubMed]
53.
Song, H.G.; Choi, I.; Choi, Y.J.; Yoon, C.S.; Han, J. High gas barrier properties of whey protein isolate-coated multi-layer film at
pilot plant facility and its application to frozen marinated meatloaf packaging. Food Packag. Shelf Life
2020
,26, 100599. [CrossRef]
54.
Böhmer-Maas, B.W.; Fonseca, L.M.; Otero, D.M.; da Rosa Zavareze, E.; Zambiazi, R.C. Photocatalytic zein-TiO2 nanofibers as
ethylene absorbers for storage of cherry tomatoes. Food Packag. Shelf Life 2020,24, 100508. [CrossRef]
55.
Xavier, L.O.; Sganzerla, W.G.; Rosa, G.B.; da Rosa, C.G.; Agostinetto, L.; Veeck, A.P.D.L.; Bretanha, L.C.; Micke, G.A.; Dalla Costa,
M.; Bertodi, F.C.; et al. Chitosan packaging functionalized with Cinnamodendron dinisii essential oil loaded zein: A proposal for
meat conservation. Int. J. Biol. Macromol. 2021,169, 183–193. [CrossRef]
56.
Amjadi, S.; Almasi, H.; Ghorbani, M.; Ramazani, S. Preparation and characterization of TiO2NPs and betanin loaded zein/sodium
alginate nanofibers. Food Packag. Shelf Life 2020,24, 100504. [CrossRef]
57.
Dong, S.; Li, X.-y.; Guo, P.; Chen, Y.; Li, H.-j. Preparation and characterization of PCL-grafted zein film via atmospheric-pressure
cold plasma pretreatment. Plasma Process. Polym. 2021,18, 2000242. [CrossRef]
58.
Ramirez, D.O.S.; Carletto, R.A.; Tonetti, C.; Giachet, F.T.; Varesano, A.; Vineis, C. Wool keratin film plasticized by citric acid for
food packaging. Food Packag. Shelf Life 2017,12, 100–106. [CrossRef]
59.
Ramakrishnan, N.; Sharma, S.; Gupta, A.; Alashwal, B.Y. Keratin based bioplastic film from chicken feathers and its characteriza-
tion. Int. J. Biol. Macromol. 2018,111, 352–358. [CrossRef]
60.
Jiang, Y.; Lan, W.T.; Sameen, D.E.; Ahmed, S.; Qin, W.; Zhang, Q.; Chen, H.; Dai, J.W.; He, L.; Liu, Y.W. Preparation and
characterization of grass carp collagen-chitosan-lemon essential oil composite films for application as food packaging. Int. J. Biol.
Macromol. 2020,160, 340–351. [CrossRef]
61.
Mangaraj, S.; Thakur, R.R.; Yadav, A. Development and characterization of PLA and Cassava starch-based novel biodegradable
film used for food packaging application. J. Food Process. Preserv. 2022,46, e16314. [CrossRef]
62.
Kostic, D.; Vukasinovic-Sekulic, M.; Armentano, I.; Torre, L.; Obradovic, B. Multifunctional ternary composite films based on PLA
and Ag/alginate microbeads: Physical characterization and silver release kinetics. Mater. Sci. Eng. C Mater. Biol. Appl.
2019
,98,
1159–1168. [CrossRef]
63.
Qiu, S.; Zhou, Y.; Waterhouse, G.I.N.; Gong, R.; Xie, J.; Zhang, K.; Xu, J. Optimizing interfacial adhesion in PBAT/PLA
nanocomposite for biodegradable packaging films. Food Chem. 2021,334, 127487. [CrossRef]
64.
Sharma, S.; Jaiswal, A.K.; Duffy, B.; Jaiswal, S. Ferulic acid incorporated active films based on poly(lactide)/poly(butylene
adipate-co-terephthalate) blend for food packaging. Food Packag. Shelf Life 2020,24, 100491. [CrossRef]
65.
Vilarinho, F.; Stanzione, M.; Buonocore, G.G.; Barbosa-Pereira, L.; Sendón, R.; Vaz, M.F.; Sanches Silva, A. Green tea extract and
nanocellulose embedded into polylactic acid film: Properties and efficiency on retarding the lipid oxidation of a model fatty food.
Food Packag. Shelf Life 2021,27, 100609. [CrossRef]
66.
Jian, J.; Xiangbin, Z.; Xianbo, H. An overview on synthesis, properties and applications of poly(butylene-adipate-co-terephthalate)–
PBAT. Adv. Ind. Eng. Polym. Res. 2020,3, 19–26. [CrossRef]
67.
Yang, C.; Tang, H.; Wang, Y.; Liu, Y.; Wang, J.; Shi, W.; Li, L. Development of PLA-PBSA based biodegradable active film and its
application to salmon slices. Food Packag. Shelf Life 2019,22, 100393. [CrossRef]
68.
Mangaraj, S.; Yadav, A.; Bal, L.M.; Dash, S.K.; Mahanti, N.K. Application of Biodegradable Polymers in Food Packaging Industry:
A Comprehensive Review. J. Packag. Technol. Res. 2018,3, 77–96. [CrossRef]
69.
Manikandan, N.A.; Pakshirajan, K.; Pugazhenthi, G. Preparation and characterization of environmentally safe and highly
biodegradable microbial polyhydroxybutyrate (PHB) based graphene nanocomposites for potential food packaging applications.
Int. J. Biol. Macromol. 2019,154, 866–877. [CrossRef]
70.
Correa, J.P.; Molina, V.; Sanchez, M.; Kainz, C.; Eisenberg, P.; Massani, M.B. Improving ham shelf life with a polyhydroxybu-
tyrate/polycaprolactone biodegradable film activated with nisin. Food Packag. Shelf Life 2017,11, 31–39. [CrossRef]
71.
Romani, V.P.; Olsen, B.; Pinto Collares, M.; Meireles Oliveira, J.R.; Prentice-Hernández, C.; Guimarães Martins, V. Improvement of
fish protein films properties for food packaging through glow discharge plasma application. Food Hydrocoll.
2019
,87, 970–976.
[CrossRef]
Foods 2023,12, 2422 54 of 59
72.
Sid, S.; Mor, R.S.; Kishore, A.; Sharanagat, V.S. Bio-sourced polymers as alternatives to conventional food packaging materials: A
review. Trends Food Sci. Technol. 2021,115, 87–104. [CrossRef]
73.
Alabi, O.A.; Ologbonjaye, K.I.; Awosolu, O.; Alalade, O.E. Public and Environmental Health Effects of Plastic Wastes Disposal: A
Review. J. Toxicol. Risk Assess. 2019,5, 021. [CrossRef]
74.
Commission Regulation. 2015/2283 of the European Parliament and of the Council of 25 November 2015 on Novel Foods,
Amending Regulation (EU) No 1169/2011 of the European Parliament and of the Council and Repealing Regulation (EC) No
258/97 of the European Parliament and of the C; 2015. Available online: https://www.legislation.gov.uk/eur/2015/2283/
contents (accessed on 6 April 2023).
75. Association of Plastic Manufacturers (Organization). Plastics—The Facts 2020; PlasticEurope: Brussels, Belgium, 2020; p. 16.
76.
European Commission. Report from the Commission to the European Parliament, the Council, the European Economic and Social
Committee and the Committee of the Regions on the Implementation of the Circular Economy Action Plan; European Commission:
Brussels, Belgium, 2019.
77.
Reichert, C.L.; Bugnicourt, E.; Coltelli, M.B.; Cinelli, P.; Lazzeri, A.; Canesi, I.; Braca, F.; Martinez, B.M.; Alonso, R.; Agostinis,
L.; et al. Bio-Based Packaging: Materials, Modifications, Industrial Applications and Sustainability. Polymers
2020
,12, 1558.
[CrossRef]
78.
European Bioplastics. Bioplastics Market Data. Available online: https://www.european-bioplastics.org/market/ (accessed on 6
April 2023).
79.
Ahmed, J.; Arfat, Y.A.; Bher, A.; Mulla, M.; Jacob, H.; Auras, R. Active Chicken Meat Packaging Based on Polylactide Films and
Bimetallic Ag–Cu Nanoparticles and Essential Oil. Food Sci. 2018,83, 1299–1310. [CrossRef]
80.
Sharma, S.; Barkauskaite, S.; Duffy, B.; Jaiswal, A.K.; Jaiswal, S. Characterization and Antimicrobial Activity of Biodegradable
Active Packaging Enriched with Clove and Thyme Essential Oil for Food Packaging Application. Foods 2020,9, 16. [CrossRef]
81.
Flórez, M.; Guerra-Rodríguez, E.; Cazón, P.; Vázquez, M. Chitosan for food packaging: Recent advances in active and intelligent
films. Food Hydrocoll. 2022,124, 107328. [CrossRef]
82.
Li, S.; Ma, Y.; Ji, T.; Sameen, D.E.; Ahmed, S.; Qin, W.; Dai, J.; Li, S.; Liu, Y. Cassava starch/carboxymethylcellulose edible films
embedded with lactic acid bacteria to extend the shelf life of banana. Carbohydr. Polym. 2020,248, 116805. [CrossRef]
83.
Jeya Jeevahan, J.; Chandrasekaran, M.; Venkatesan, S.P.; Sriram, V.; Britto Joseph, G.; Mageshwaran, G.; Durairaj, R.B. Scaling up
difficulties and commercial aspects of edible films for food packaging: A review. Trends Food Sci. Technol.
2020
,100, 210–222.
[CrossRef]
84.
Caroline da Silva Rocha, A.; Rodrigues Menezes, L.; Silva, E.O.d.; Pedrosa, M.C.G. Synergistic effect of carbon nanoparticles
on the mechanical and thermal properties of poly(lactic acid) as promising systems for packaging. J. Compos. Mater.
2020
,54,
4133–4144. [CrossRef]
85.
Wróblewska-Krepsztul, J.; Rydzkowski, T.; Borowski, G.; Szczypi´nski, M.; Klepka, T.; Thakur, V.K. Recent progress in biodegrad-
able polymers and nanocomposite-based packaging materials for sustainable environment. Int. J. Polym. Anal. Charact.
2018
,23,
383–395. [CrossRef]
86.
Siracusa, V.; Rocculi, P.; Romani, S.; Rosa, M.D. Biodegradable polymers for food packaging: A review. Trends Food Sci. Technol.
2008,19, 634–643. [CrossRef]
87.
Lee, H.; Rukmanikrishnan, B.; Lee, J. Rheological, morphological, mechanical, and water-barrier properties of agar/gellan
gum/montmorillonite clay composite films. Int. J. Biol. Macromol. 2019,141, 538–544. [CrossRef] [PubMed]
88.
Polman, E.M.N.; Gruter, G.M.; Parsons, J.R.; Tietema, A. Comparison of the aerobic biodegradation of biopolymers and the
corresponding bioplastics: A review. Sci. Total Environ. 2021,753, 141953. [CrossRef] [PubMed]
89.
Ahsan, W.A.; Hussain, A.; Lin, C.; Nguyen, M.K. Biodegradation of Different Types of Bioplastics through Composting—A
Recent Trend in Green Recycling. Catalysts 2023,13, 294. [CrossRef]
90.
Pires, J.R.A.; Souza, V.G.L.; Fuciños, P.; Pastrana, L.; Fernando, A.L. Methodologies to Assess the Biodegradability of Bio-Based
Polymers—Current Knowledge and Existing Gaps. Polymers 2022,14, 1359.
91.
Wang, J.; Gardner, D.J.; Stark, N.M.; Bousfield, D.W.; Tajvidi, M.; Cai, Z. Moisture and Oxygen Barrier Properties of Cellulose
Nanomaterial-Based Films. ACS Sustain. Chem. Eng. 2018,6, 49–70. [CrossRef]
92.
Roy, S.; Rhim, J.-W.; Jaiswal, L. Bioactive agar-based functional composite film incorporated with copper sulfide nanoparticles.
Food Hydrocoll. 2019,93, 156–166. [CrossRef]
93.
Rukmanikrishnan, B.; Ramalingam, S.; Rajasekharan, S.K.; Lee, J.; Lee, J. Binary and ternary sustainable composites of gellan
gum, hydroxyethyl cellulose and lignin for food packaging applications: Biocompatibility, antioxidant activity, UV and water
barrier properties. Int. J. Biol. Macromol. 2020,153, 55–62. [CrossRef]
94.
Mathew, S.; Snigdha, S.; Mathew, J.; Radhakrishnan, E.K. Biodegradable and active nanocomposite pouches reinforced with silver
nanoparticles for improved packaging of chicken sausages. Food Packag. Shelf Life 2019,19, 155–166. [CrossRef]
95.
Mohamed, S.A.A.; El-Sakhawy, M.; El-Sakhawy, M.A.M. Polysaccharides, Protein and Lipid -Based Natural Edible Films in Food
Packaging: A Review. Carbohydr. Polym. 2020,238, 116178. [CrossRef]
96.
Cao, W.; Yan, J.; Liu, C.; Zhang, J.; Wang, H.; Gao, X.; Yan, H.; Niu, B.; Li, W. Preparation and characterization of catechol-grafted
chitosan/gelatin/modified chitosan-AgNP blend films. Carbohydr. Polym. 2020,247, 116643. [CrossRef]
97.
Huang, G.; Chen, F.; Yang, W.; Huang, H. Preparation, deproteinization and comparison of bioactive polysaccharides. Trends Food
Sci. Technol. 2021,109, 564–568. [CrossRef]
Foods 2023,12, 2422 55 of 59
98.
Mohamad, N.; Mazlan, M.M.; Tawakkal, I.S.M.A.; Talib, R.A.; Kian, L.K.; Fouad, H.; Jawaid, M. Development of active agents
filled polylactic acid films for food packaging application. Int. J. Biol. Macromol. 2020,163, 1451–1457. [CrossRef] [PubMed]
99.
Zhang, J.; Xu, W.R.; Zhang, Y.C.; Han, X.D.; Chen, C.; Chen, A. In situ generated silica reinforced polyvinyl alcohol/liquefied
chitin biodegradable films for food packaging. Carbohydr. Polym. 2020,238, 116182. [CrossRef] [PubMed]
100.
Zhou, X.; Ye, X.; He, J.; Wang, R.; Jin, Z. Effects of electron beam irradiation on the properties of waxy maize starch and its films.
Int. J. Biol. Macromol. 2020,151, 239–246. [CrossRef]
101.
Zheng, Q.; Tian, Y.; Ye, F.; Zhou, Y.; Zhao, G. Fabrication and application of starch-based aerogel: Technical strategies. Trends Food
Sci. Technol. 2020,99, 608–620. [CrossRef]
102.
Chi, K.; Wang, H.; Catchmark, J.M. Sustainable starch-based barrier coatings for packaging applications. Food Hydrocoll.
2020
,
103, 105696. [CrossRef]
103.
Chaireh, S.; Ngasatool, P.; Kaewtatip, K. Novel composite foam made from starch and water hyacinth with beeswax coating for
food packaging applications. Int. J. Biol. Macromol. 2020,165, 1382–1391. [CrossRef]
104.
Zhang, K.; Su, T.; Cheng, F.; Lin, Y.; Zhou, M.; Zhu, P.; Li, R.; Wu, D. Effect of sodium citrate/polyethylene glycol on plasticization
and retrogradation of maize starch. Int. J. Biol. Macromol. 2020,154, 1471–1477. [CrossRef]
105.
Tibolla, H.; Czaikoski, A.; Pelissari, F.M.; Menegalli, F.C.; Cunha, R.L. Starch-based nanocomposites with cellulose nanofibers
obtained from chemical and mechanical treatments. Int. J. Biol. Macromol. 2020,161, 132–146. [CrossRef]
106.
Othman, S.H.; Wane, B.M.; Nordin, N.; Noor Hasnan, N.Z.; ATalib, R.; Karyadi, J.N.W. Physical, Mechanical, and Water Vapor
Barrier Properties of Starch/Cellulose Nanofiber/Thymol Bionanocomposite Films. Polymers
2021
,13, 4060. [CrossRef] [PubMed]
107.
Cheng, M.; Cui, Y.; Yan, X.; Zhang, R.; Wang, J.; Wang, X. Effect of dual-modified cassava starches on intelligent packaging films
containing red cabbage extracts. Food Hydrocoll. 2022,124, 107225. [CrossRef]
108.
Lan, W.; Zhang, R.; Ji, T.; Sameen, D.E.; Ahmed, S.; Qin, W.; Dai, J.; He, L.; Liu, Y. Improving nisin production by encapsulated
Lactococcus lactis with starch/carboxymethyl cellulose edible films. Carbohydr. Polym. 2021,251, 117062. [CrossRef] [PubMed]
109.
Merz, B.; Capello, C.; Leandro, G.C.; Moritz, D.E.; Monteiro, A.R.; Valencia, G.A. A novel colorimetric indicator film based on
chitosan, polyvinyl alcohol and anthocyanins from jambolan (Syzygium cumini) fruit for monitoring shrimp freshness. Int. J. Biol.
Macromol. 2020,153, 625–632. [CrossRef]
110.
Indumathi, M.P.; Sarojini, K.S.; Rajarajeswari, G.R. Antimicrobial and biodegradable chitosan/cellulose acetate phthalate/ZnO
nano composite films with optimal oxygen permeability and hydrophobicity for extending the shelf life of black grape fruits. Int.
J. Biol. Macromol. 2019,132, 1112–1120. [CrossRef]
111.
Kaewklin, P.; Siripatrawan, U.; Suwanagul, A.; Lee, Y.S. Active packaging from chitosan-titanium dioxide nanocomposite film for
prolonging storage life of tomato fruit. Int. J. Biol. Macromol. 2018,112, 523–529. [CrossRef]
112.
Hosseinzadeh, S.; Partovi, R.; Talebi, F.; Babaei, A. Chitosan/TiO
2
nanoparticle/Cymbopogon citratus essential oil film as food
packaging material: Physico-mechanical properties and its effects on microbial, chemical, and organoleptic quality of minced
meat during refrigeration. J. Food Process. Preserv. 2020,44, e14536. [CrossRef]
113.
Gasti, T.; Dixit, S.; Hiremani, V.D.; Chougale, R.B.; Masti, S.P.; Vootla, S.K.; Mudigoudra, B.S. Chitosan/pullulan based films
incorporated with clove essential oil loaded chitosan-ZnO hybrid nanoparticles for active food packaging. Carbohydr. Polym.
2022,277, 118866. [CrossRef]
114.
Dong, W.; Su, J.; Chen, Y.; Xu, D.; Cheng, L.; Mao, L.; Gao, Y.; Yuan, F. Characterization and antioxidant properties of chitosan
film incorporated with modified silica nanoparticles as an active food packaging. Food Chem. 2022,373, 131414. [CrossRef]
115.
Li, F.; Liu, Y.N.; Cao, Y.Y.; Zhang, Y.L.; Zhe, T.T.; Guo, Z.R.; Sun, X.Y.; Wang, Q.Z.; Wang, L. Copper sulfide nanoparticle-
carrageenan films for packaging application. Food Hydrocoll. 2020,109, 106094. [CrossRef]
116.
Liu, Y.; Zhang, X.; Li, C.; Qin, Y.; Xiao, L.; Liu, J. Comparison of the structural, physical and functional properties of
κ
-carrageenan
films incorporated with pomegranate flesh and peel extracts. Int. J. Biol. Macromol. 2020,147, 1076–1088. [CrossRef] [PubMed]
117.
Yadav, M.; Chiu, F.C. Cellulose nanocrystals reinforced
κ
-carrageenan based UV resistant transparent bionanocomposite films for
sustainable packaging applications. Carbohydr. Polym. 2019,211, 181–194. [CrossRef] [PubMed]
118.
Alizadeh Sani, M.; Tavassoli, M.; Salim, S.A.; Azizi-lalabadi, M.; McClements, D.J. Development of green halochromic smart
and active packaging materials: TiO
2
nanoparticle- and anthocyanin-loaded gelatin/
κ
-carrageenan films. Food Hydrocoll.
2022
,
124, 107324. [CrossRef]
119.
Velásquez, P.; Montenegro, G.; Valenzuela, L.M.; Giordano, A.; Cabrera-Barjas, G.; Martin-Belloso, O.
κ
-carrageenan edible
films for beef: Honey and bee pollen phenolic compounds improve their antioxidant capacity. Food Hydrocoll. 2022,124, 107250.
[CrossRef]
120.
da Silva Filipini, G.; Romani, V.P.; Guimarães Martins, V. Biodegradable and active-intelligent films based on methylcellulose and
jambolão (Syzygium cumini) skins extract for food packaging. Food Hydrocoll. 2020,109, 106139. [CrossRef]
121.
Tavares, K.M.; Campos, A.D.; Luchesi, B.R.; Resende, A.A.; Oliveira, J.E.D.; Marconcini, J.M. Effect of carboxymethyl cellulose
concentration on mechanical and water vapor barrier properties of corn starch films. Carbohydr. Polym.
2020
,246, 116521.
[CrossRef]
122.
Saedi, S.; Shokri, M.; Kim, J.T.; Shin, G.H. Semi-transparent regenerated cellulose/ZnONP nanocomposite film as a potential
antimicrobial food packaging material. J. Food Eng. 2021,307, 110665. [CrossRef]
Foods 2023,12, 2422 56 of 59
123.
Atta, O.M.; Manan, S.; Ahmed, A.A.Q.; Awad, M.F.; Ul-Islam, M.; Subhan, F.; Ullah, M.W.; Yang, G. Development and
Characterization of Yeast-Incorporated Antimicrobial Cellulose Biofilms for Edible Food Packaging Application. Polymer.
2021
,
13, 2310. [CrossRef]
124.
Zhang, R.; Zhai, X.; Wang, W.; Hou, H. Preparation and evaluation of agar/maltodextrin-beeswax emulsion films with various
hydrophilic-lipophilic balance emulsifiers. Food Chem. 2022,384, 132541. [CrossRef]
125.
Hong, S.-I.; Cho, Y.; Rhim, J.-W. Effect of Agar/AgNP Composite Film Packaging on Refrigerated Beef Loin Quality. Membranes
2021,11, 750. [CrossRef] [PubMed]
126.
Hashim, S.B.H.; Elrasheid Tahir, H.; Liu, L.; Zhang, J.; Zhai, X.; Ali Mahdi, A.; Nureldin Awad, F.; Hassan, M.M.; Xiaobo, Z.;
Jiyong, S. Intelligent colorimetric pH sensoring packaging films based on sugarcane wax/agar integrated with butterfly pea
flower extract for optical tracking of shrimp freshness. Food Chem. 2022,373, 131514. [CrossRef] [PubMed]
127.
Dash, K.K.; Ali, N.A.; Das, D.; Mohanta, D. Thorough evaluation of sweet potato starch and lemon-waste pectin based-edible
films with nano-titania inclusions for food packaging applications. Int. J. Biol. Macromol.
2019
,139, 449–458. [CrossRef] [PubMed]
128.
Han, H.-S.; Song, K.B. Antioxidant properties of watermelon (Citrullus lanatus) rind pectin films containing kiwifruit (Actinidia
chinensis) peel extract and their application as chicken thigh packaging. Food Packag. Shelf Life 2021,28, 100636. [CrossRef]
129.
Roy, S.; Rhim, J.-W. Preparation of pectin/agar-based functional films integrated with zinc sulfide nano petals for active packaging
applications. Colloids Surf. B Biointerfaces 2021,207, 111999. [CrossRef]
130.
Singh, P.; Baisthakur, P.; Yemul, O.S. Synthesis, characterization and application of crosslinked alginate as green packaging
material. Heliyon 2020,6, e03026. [CrossRef]
131.
Vizzini, P.; Beltrame, E.; Zanet, V.; Vidic, J.; Manzano, M. Development and Evaluation of qPCR Detection Method and Zn-
MgO/Alginate Active Packaging for Controlling Listeria monocytogenes Contamination in Cold-Smoked Salmon. Foods
2020
,
9, 1353. [CrossRef]
132.
Saravanakumar, K.; Sathiyaseelan, A.; Mariadoss, A.V.A.; Hu, X.W.; Wang, M.H. Physical and bioactivities of biopolymeric films
incorporated with cellulose, sodium alginate and copper oxide nanoparticles for food packaging application. Int. J. Biol. Macromol.
2020,153, 207–214. [CrossRef]
133.
Abdel Aziz, M.S.; Salama, H.E. Developing multifunctional edible coatings based on alginate for active food packaging. Int. J.
Biol. Macromol. 2021,190, 837–844. [CrossRef]
134.
Priyadarshi, R.; Kim, H.-J.; Rhim, J.-W. Effect of sulfur nanoparticles on properties of alginate-based films for active food
packaging applications. Food Hydrocoll. 2021,110, 106155. [CrossRef]
135.
Mohsin, A.; Zaman, W.Q.; Guo, M.; Ahmed, W.; Khan, I.M.; Niazi, S.; Rehman, A.; Hang, H.; Zhuang, Y. Xanthan-Curdlan nexus
for synthesizing edible food packaging films. Int. J. Biol. Macromol. 2020,162, 43–49. [CrossRef]
136.
Wei, Y.C.; Cheng, C.H.; Ho, Y.C.; Tsai, M.L.; Mi, F.L. Active gellan gum/purple sweet potato composite films capable of monitoring
pH variations. Food Hydrocoll. 2017,69, 491–502. [CrossRef]
137.
Goudar, N.; Vanjeri, V.N.; Dixit, S.; Hiremani, V.; Sataraddi, S.; Gasti, T.; Vootla, S.K.; Masti, S.P.; Chougale, R.B. Evaluation
of multifunctional properties of gallic acid crosslinked Poly (vinyl alcohol)/Tragacanth Gum blend films for food packaging
applications. Int. J. Biol. Macromol. 2020,158, 139–149. [CrossRef] [PubMed]
138.
Silva, N.H.C.S.; Vilela, C.; Almeida, A.; Marrucho, I.M.; Freire, C.S.R. Pullulan-based nanocomposite films for functional food
packaging: Exploiting lysozyme nanofibers as antibacterial and antioxidant reinforcing additives. Food Hydrocoll.
2018
,77,
921–930. [CrossRef]
139.
Han, K.; Liu, Y.; Liu, Y.; Huang, X.; Sheng, L. Characterization and film-forming mechanism of egg white/pullulan blend film.
Food Chem. 2020,315, 126201. [CrossRef] [PubMed]
140.
Shanmugam, R.; Mayakrishnan, V.; Kesavan, R.; Shanmugam, K.; Veeramani, S.; Ilangovan, R. Mechanical, Barrier, Adhesion
and Antibacterial Properties of Pullulan/Graphene Bio Nanocomposite Coating on Spray Coated Nanocellulose Film for Food
Packaging Applications. J. Polym. Environ. 2022,30, 1749–1757. [CrossRef]
141.
Khan, M.J.; Ramiah, S.K.; Selamat, J.; Shameli, K.; Sazili, A.Q.; Mookiah, S. Utilisation of pullulan active packaging incorporated
with curcumin and pullulan mediated silver nanoparticles to maintain the quality and shelf life of broiler meat. Ital. J. Anim. Sci.
2022,21, 244–262. [CrossRef]
142.
Chen, F.; Chi, C. Development of pullulan/carboxylated cellulose nanocrystal/tea polyphenol bionanocomposite films for active
food packaging. Int. J. Biol. Macromol. 2021,186, 405–413. [CrossRef]
143.
Duan, M.; Yu, S.; Sun, J.; Jiang, H.; Zhao, J.; Tong, C.; Hu, Y.; Pang, J.; Wu, C. Development and characterization of electrospun
nanofibers based on pullulan/chitin nanofibers containing curcumin and anthocyanins for active-intelligent food packaging. Int.
J. Biol. Macromol. 2021,187, 332–340. [CrossRef]
144. Gniewosz, M.; Pobiega, K.; Kra´sniewska, K.; Synowiec, A.; Chaberek, M.; Galus, S. Characterization and Antifungal Activity of
Pullulan Edible Films Enriched with Propolis Extract for Active Packaging. Foods 2022,11, 2319. [CrossRef]
145.
Ceballos, R.L.; Ochoa-Yepes, O.; Goyanes, S.; Bernal, C.; Fama, L. Effect of yerba mate extract on the performance of starch films
obtained by extrusion and compression molding as active and smart packaging. Carbohydr. Polym.
2020
,244, 116495. [CrossRef]
[PubMed]
146.
Wang, Y.B.; Cen, C.N.; Chen, J.; Fu, L.L. MgO/carboxymethyl chitosan nanocomposite improves thermal stability, waterproof
and antibacterial performance for food packaging. Carbohydr. Polym. 2020,236, 116078. [CrossRef] [PubMed]
Foods 2023,12, 2422 57 of 59
147.
Li, K.; Zhu, J.; Guan, G.; Wu, H. Preparation of chitosan-sodium alginate films through layer-by-layer assembly and ferulic acid
crosslinking: Film properties, characterization, and formation mechanism. Int. J. Biol. Macromol.
2019
,122, 485–492. [CrossRef]
[PubMed]
148.
Hasan, M.; Rusman, R.; Khaldun, I.; Ardana, L.; Mudatsir, M.; Fansuri, H. Active edible sugar palm starch-chitosan films carrying
extra virgin olive oil: Barrier, thermo-mechanical, antioxidant, and antimicrobial properties. Int. J. Biol. Macromol.
2020
,163,
766–775. [CrossRef]
149.
Younis, H.G.R.; Zhao, G. Physicochemical properties of the edible films from the blends of high methoxyl apple pectin and
chitosan. Int. J. Biol. Macromol. 2019,131, 1057–1066. [CrossRef]
150.
de Moraes Crizel, T.; de Oliveira Rios, A.; Alves, V.D.; Bandarra, N.; Moldão-Martins, M.; Flôres, S.H. Active food packaging
prepared with chitosan and olive pomace. Food Hydrocoll. 2018,74, 139–150. [CrossRef]
151.
Yong, H.; Wang, X.; Bai, R.; Miao, Z.; Zhang, X.; Liu, J. Development of antioxidant and intelligent pH-sensing packaging films by
incorporating purple-fleshed sweet potato extract into chitosan matrix. Food Hydrocoll. 2019,90, 216–224. [CrossRef]
152.
Riaz, A.; Lei, S.; Akhtar, H.M.S.; Wan, P.; Chen, D.; Jabbar, S.; Abid, M.; Hashim, M.M.; Zeng, X. Preparation and characterization
of chitosan-based antimicrobial active food packaging film incorporated with apple peel polyphenols. Int. J. Biol. Macromol.
2018
,
114, 547–555. [CrossRef]
153.
Wang, X.; Yong, H.; Gao, L.; Li, L.; Jin, M.; Liu, J. Preparation and characterization of antioxidant and pH-sensitive films based on
chitosan and black soybean seed coat extract. Food Hydrocoll. 2019,89, 56–66. [CrossRef]
154.
Riaz, A.; Lagnika, C.; Luo, H.; Dai, Z.; Nie, M.; Hashim, M.M.; Liu, C.; Song, J.; Li, D. Chitosan-based biodegradable active food
packaging film containing Chinese chive (Allium tuberosum) root extract for food application. Int. J. Biol. Macromol.
2020
,150,
595–604. [CrossRef]
155.
do Vale, D.A.; Vieira, C.B.; Vidal, M.F.; Claudino, R.L.; Andrade, F.K.; Sousa, J.R.; Souza Filho, M.d.S.M.; da Silva, A.L.C.; de
Souza, B.W.S. Chitosan-Based Edible Films Produced from Crab-Uçá(Ucides cordatus) Waste: Physicochemical, Mechanical and
Antimicrobial Properties. J. Polym. Environ. 2021,29, 694–706. [CrossRef]
156.
Lin, D.R.; Yang, Y.M.; Wang, J.; Yan, W.J.; Wu, Z.J.; Chen, H.; Zhang, Q.; Wu, D.T.; Qin, W.; Tu, Z.C. Preparation and characterization
of TiO2-Ag loaded fish gelatin-chitosan antibacterial composite film for food packaging. Int. J. Biol. Macromol.
2020
,154, 123–133.
[CrossRef] [PubMed]
157.
Panariello, L.; Coltelli, M.-B.; Buchignani, M.; Lazzeri, A. Chitosan and nano-structured chitin for biobased anti-microbial
treatments onto cellulose based materials. Eur. Polym. 2019,113, 328–339. [CrossRef]
158.
Sun, G.; Chi, W.; Zhang, C.; Xu, S.; Li, J.; Wang, L. Developing a green film with pH-sensitivity and antioxidant activity based
on
κ
-carrageenan and hydroxypropyl methylcellulose incorporating Prunus maackii juice. Food Hydrocoll.
2019
,94, 345–353.
[CrossRef]
159.
Wang, R.; Li, X.; Ren, Z.; Xie, S.; Wu, Y.; Chen, W.; Ma, F.; Liu, X. Characterization and antibacterial properties of biodegradable
films based on CMC, mucilage from Dioscorea opposita Thunb. and Ag nanoparticles. Int. J. Biol. Macromol.
2020
,163, 2189–2198.
[CrossRef] [PubMed]
160.
Sá, N.M.S.M.; Mattos, A.L.A.; Silva, L.M.A.; Brito, E.S.; Rosa, M.F.; Azeredo, H.M.C. From cashew byproducts to biodegradable
active materials: Bacterial cellulose-lignin-cellulose nanocrystal nanocomposite films. Int. J. Biol. Macromol.
2020
,161, 1337–1345.
[CrossRef] [PubMed]
161.
Zhang, R.; Wang, W.; Zhang, H.; Dai, Y.; Dong, H.; Kong, L.; Hou, H. Effects of preparation conditions on the properties of
agar/maltodextrin-beeswax pseudo-bilayer films. Carbohydr. Polym. 2020,236, 116029. [CrossRef]
162. Kontominas, M.G. Use of Alginates as Food Packaging Materials. Foods 2020,9, 1440. [CrossRef]
163.
Mohammadi, M.; Mirabzadeh, S.; Shahvalizadeh, R.; Hamishehkar, H. Development of novel active packaging films based on
whey protein isolate incorporated with chitosan nanofiber and nano-formulated cinnamon oil. Int. J. Biol. Macromol.
2020
,149,
11–20. [CrossRef]
164.
Liu, Y.; Wang, D.; Sun, Z.; Liu, F.; Du, L.; Wang, D. Preparation and characterization of gelatin/chitosan/3-phenylacetic acid
food-packaging nanofiber antibacterial films by electrospinning. Int. J. Biol. Macromol. 2021,169, 161–170. [CrossRef]
165.
Ge, Y.; Li, Y.; Bai, Y.; Yuan, C.; Wu, C.; Hu, Y. Intelligent gelatin/oxidized chitin nanocrystals nanocomposite films containing
black rice bran anthocyanins for fish freshness monitorings. Int. J. Biol. Macromol. 2020,155, 1296–1306. [CrossRef] [PubMed]
166.
Xin, S.; Xiao, L.; Dong, X.; Li, X.; Wang, Y.; Hu, X.; Sameen, D.E.; Qin, W.; Zhu, B. Preparation of chitosan/curcumin nanoparticles
based zein and potato starch composite films for Schizothorax prenati fillet preservation. Int. J. Biol. Macromol.
2020
,164, 211–221.
[CrossRef] [PubMed]
167.
Cui, H.Y.; Surendhiran, D.; Li, C.Z.; Lin, L. Biodegradable zein active film containing chitosan nanoparticle encapsulated with
pomegranate peel extract for food packaging. Food Packag. Shelf Life 2020,24, 100511. [CrossRef]
168.
Oluba, O.M.; Obi, C.F.; Akpor, O.B.; Ojeaburu, S.I.; Ogunrotimi, F.D.; Adediran, A.A.; Oki, M. Fabrication and characterization of
keratin starch biocomposite film from chicken feather waste and ginger starch. Sci. Rep. 2021,11, 8768. [CrossRef]
169.
Marangoni Júnior, L.; Silva, R.G.d.; Vieira, R.P.; Alves, R.M.V. Water vapor sorption and permeability of sustainable algi-
nate/collagen/SiO2 composite films. LWT 2021,152, 112261. [CrossRef]
Foods 2023,12, 2422 58 of 59
170.
Figueroa-Lopez, K.J.; Torres-Giner, S.; Angulo, I.; Pardo-Figuerez, M.; Escuin, J.M.; Bourbon, A.I.; Cabedo, L.; Nevo, Y.; Cerqueira,
M.A.; Lagaron, J.M. Development of active barrier multilayer films based on electrospun antimicrobial hot-tack food waste
derived poly(3-hydroxybutyrate-co-3-hydroxyvalerate) and cellulose nanocrystal interlayers. Nanomaterials
2020
,10, 2356.
[CrossRef]
171.
Roy, S.; Ezati, P.; Rhim, J.-W. Gelatin/Carrageenan-Based Functional Films with Carbon Dots from Enoki Mushroom for Active
Food Packaging Applications. ACS Appl. Polym. Mater. 2021,3, 6437–6445. [CrossRef]
172.
Roy, S.; Rhim, J.W. Preparation of Gelatin/Carrageenan-Based Color-Indicator Film Integrated with Shikonin and Propolis for
Smart Food Packaging Applications. ACS Appl. Bio Mater. 2021,4, 770–779. [CrossRef]
173.
Lan, X.; Luo, T.; Zhong, Z.; Huang, D.; Liang, C.; Liu, Y.; Wang, H.; Tang, Y. Green cross-linking of gelatin/tea polyphenol/
ε
-poly
(L-lysine) electrospun nanofibrous membrane for edible and bioactive food packaging. Food Packag. Shelf Life
2022
,34, 100970.
[CrossRef]
174.
Dou, Y.; Zhang, L.; Zhang, B.; He, M.; Shi, W.; Yang, S.; Cui, Y.; Yin, G. Preparation and Characterization of Edible Dialdehyde
Carboxymethyl Cellulose Crosslinked Feather Keratin Films for Food Packaging. Polymers 2020,12, 158. [CrossRef]
175.
Wei, L.; Zhu, S.; Yang, H.; Liao, Z.; Gong, Z.; Zhao, W.; Li, Y.; Gu, J.; Wei, Z.; Yang, J. Keratin-Based Composite Bioactive Films and
Their Preservative Effects on Cherry Tomato. Molecules 2022,27, 6331. [CrossRef] [PubMed]
176.
Lara, B.R.B.; de Andrade, P.S.; Guimarães Junior, M.; Dias, M.V.; Alcântara, L.A.P. Novel Whey Protein Isolate/Polyvinyl
Biocomposite for Packaging: Improvement of Mechanical and Water Barrier Properties by Incorporation of Nano-silica. J. Polym.
Environ. 2021,29, 2397–2408. [CrossRef]
177.
Jiang, L.; Liu, F.; Wang, F.; Zhang, H.; Kang, M. Development and characterization of zein-based active packaging films containing
catechin loaded β-cyclodextrin metal-organic frameworks. Food Packag. Shelf Life 2022,31, 100810. [CrossRef]
178.
Andrade-Del Olmo, J.; Pérez-Álvarez, L.; Hernáez, E.; Ruiz-Rubio, L.; Vilas-Vilela, J.L. Antibacterial multilayer of chitosan and
(2-carboxyethyl)- β-cyclodextrin onto polylactic acid (PLLA). Food Hydrocoll. 2019,88, 228–236. [CrossRef]
179.
Arumugam, S.; Kandasamy, J.; Thiyaku, T.; Saxena, P. Effect of Low Concentration of SiO2 Nanoparticles on Grape Seed Essential
Oil/PBAT Composite Films for Sustainable Food Packaging Application. Sustainability 2022,14, 8073. [CrossRef]
180.
Lukic, I.; Vulic, J.; Ivanovic, J. Antioxidant activity of PLA/PCL films loaded with thymol and/or carvacrol using scCO2 for
active food packaging. Food Packag. Shelf Life 2020,26, 100578. [CrossRef]
181.
Diken, M.E.; Koçer Kizilduman, B.; Do ˘gan, S.; Do ˘gan, M. Antibacterial and antioxidant phenolic compounds loaded PCL
biocomposites for active food packaging application. J. Appl. Polym. Sci. 2022,139, e52423. [CrossRef]
182.
Melendez-Rodriguez, B.; Torres-Giner, S.; Angulo, I.; Pardo-Figuerez, M.; Hilliou, L.; Escuin, J.M.; Cabedo, L.; Nevo, Y.; Prieto, C.;
Lagaron, J.M. High-Oxygen-Barrier Multilayer Films Based on Polyhydroxyalkanoates and Cellulose Nanocrystals. Nanomaterials
2021,11, 1443. [CrossRef]
183.
Zhang, X.; Wang, H.; Niu, N.; Chen, Z.; Li, S.; Liu, S.-X.; Li, J. Fluorescent Poly(vinyl alcohol) Films Containing Chlorogenic Acid
Carbon Nanodots for Food Monitoring. ACS Appl. Nano Mater. 2020,3, 7611–7620. [CrossRef]
184. Yang, W.; Weng, Y.; Puglia, D.; Qi, G.; Dong, W.; Kenny, J.M.; Ma, P. Poly(lactic acid)/lignin films with enhanced toughness and
anti-oxidation performance for active food packaging. Int. J. Biol. Macromol. 2020,144, 102–110. [CrossRef]
185.
Akshaykranth, A.; Jayarambabu, N.; Venkatappa Rao, T.; Rakesh Kumar, R.; Srinivasa Rao, L. Antibacterial activity study of ZnO
incorporated biodegradable poly (lactic acid) films for food packaging applications. Polym. Bull.
2023
,80, 1369–1384. [CrossRef]
186.
Subbuvel, M.; Kavan, P. Preparation and characterization of polylactic acid/fenugreek essential oil/curcumin composite films for
food packaging applications. Int. J. Biol. Macromol. 2022,194, 470–483. [CrossRef] [PubMed]
187.
Sharma, S.; Perera, K.Y.; Pradhan, D.; Duffy, B.; Jaiswal, A.K.; Jaiswal, S. Active Packaging Film Based on Poly Lactide-Poly
(Butylene Adipate-Co-Terephthalate) Blends Incorporated with Tannic Acid and Gallic Acid for the Prolonged Shelf Life of
Cherry Tomato. Coatings 2022,12, 1902. [CrossRef]
188.
Marzano-Barreda, L.A.; Yamashita, F.; Bilck, A.P. Effect of biodegradable active packaging with zeolites on fresh broccoli florets. J.
Food Sci. Technol. 2021,58, 197–204. [CrossRef]
189.
Klinmalai, P.; Srisa, A.; Laorenza, Y.; Katekhong, W.; Harnkarnsujarit, N. Antifungal and plasticization effects of carvacrol in
biodegradable poly(lactic acid) and poly(butylene adipate terephthalate) blend films for bakery packaging. LWT
2021
,152, 112356.
[CrossRef]
190.
Charoensri, K.; Rodwihok, C.; Ko, S.H.; Wongratanaphisan, D.; Park, H.J. Enhanced antimicrobial and physical properties of poly
(butylene adipate-co-terephthalate)/zinc oxide/reduced graphene oxide ternary nanocomposite films. Mater. Today Commun.
2021,28, 102586. [CrossRef]
191.
Dumitriu, R.P.; Stoleru, E.; Mitchell, G.R.; Vasile, C.; Brebu, M. Bioactive Electrospun Fibers of Poly(
ε
-Caprolactone) Incorporating
α-Tocopherol for Food Packaging Applications. Molecules 2021,26, 5498. [CrossRef]
192.
Cheng, P.-f.; Liang, M.; Yun, X.-y.; Dong, T. Biodegradable blend films of poly(
ε
-caprolactone)/poly(propylene carbonate) for
shelf life extension of whole white button mushrooms. J. Food Sci. Technol. 2022,59, 144–156. [CrossRef]
193.
Rech, C.R.; Brabes, K.C.S.; Silva, B.E.B.; Martines, M.A.U.; Silveira, T.F.S.; Alberton, J.; Amadeu, C.A.A.; Caon, T.; Arruda, E.J.;
Martelli, S.M. Antimicrobial and Physical–Mechanical Properties of Polyhydroxybutyrate Edible Films Containing Essential Oil
Mixtures. J. Polym. Environ. 2021,29, 1202–1211. [CrossRef]
Foods 2023,12, 2422 59 of 59
194.
Le Delliou, B.; Vitrac, O.; Castro, M.; Bruzaud, S.; Domenek, S. Characterization of a new bio-based and biodegradable blends of
poly(3-hydroxybutyrate-co-3-hydroxyvalerate) and poly(butylene-co-succinate-co-adipate). J. Appl. Polym. Sci.
2022
,139, 52124.
[CrossRef]
195.
La Fuente Arias, C.I.; González-Martínez, C.; Chiralt, A. Lamination of starch/polyesters by thermocompression for food
packaging purposes. Sustain. Food Technol. 2023,1, 296–305. [CrossRef]
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