Access to this full-text is provided by De Gruyter.
Content available from Nanotechnology Reviews
This content is subject to copyright. Terms and conditions apply.
Research Article
Razali M. O. Syafiq, Salit M. Sapuan*, and Mohd R. M. Zuhri
Effect of cinnamon essential oil on morphological, flammability
and thermal properties of nanocellulose fibre–reinforced starch
biopolymer composites
https://doi.org/10.1515/ntrev-2020-0087
received September 26, 2020; accepted October 8, 2020
Abstract: The effect of different cinnamon essential oil
(CEO)contents on flammability, thermal stability and
morphological characteristics of nanocellulose fibre–
reinforced starch biopolymer composites was studied.
This sugar palm nanocellulose reinforced with sugar
palm starch, containing 0–2% CEO, was prepared through
solution casting technique. From scanning electron micro-
scopy analysis, the cross-sections of the CEO-containing
films showed appearance of micro-porous spots as
micro-porous holes because of the occurrence of partial
evaporation on the cryo-fractured surface as a result of
the vacuum condition. Increment in CEO concentration
resulted in increasing trend of the number and size
of the micro-porous holes. Significant increase was
observed in the thermal stability with the CEO loading
when compared with neat composites. Besides that,
increasing CEO loading also resulted in decrement of
linear burning rate of the composites.
Keywords: morphological properties, flammability, sugar
palm nanocellulose, sugar palm starch, essential oil
1 Introduction
Conventional packaging from petroleum-based plastics,
such as polypropylene, polyethylene, polyvinyl chloride,
polyamide, polyethylene terephthalate and high density
polyethylene, is being extensivelyusedinfoodandbeverage
industries considering their ease of processing, strength, cost
effectiveness and durability [1,2]. Food packaging requires a
considerable consumption of various materials, where
utilization of plastics has exponentially increased over
the last two decades, with approximately 5% annual
growth. Plastics, after paper and cardboard, are also the
second most regularly used materials in food packaging
applications. According to Sanyang et al. [3],thelackof
biodegradability of conventional packaging materials that
are petroleum based is known to contribute to many
environmental hazards, e.g. emitting dangerous toxins
into the air and destroying ocean habitats from the coral
reefs to thousands of other species. This will lead to loss
of revenue for fishing and tourism industries. Moreover,
restoring it is costly as the cities, states and country need
to spend millions of their revenues to clear-out littered
plastics as well as to build and sustain landfills.
In recent years, biodegradable polymers, particularly
agro-based polymers, have been widely explored as alter-
natives to non-degradable polymers that are now primarily
used in the production of food packaging films [4–7].Starch
is one of the widest packaging biopolymers available as it is
easily available, biodegradable, renewable and of low cost
[8,9]. Therefore, starch has drawn considerable interests
as an alternative to non-biodegradable plastics, hence a
promising new green material in the industry [10].How-
ever, starch-based films for packaging applications have
reportedly shown that they have poor antimicrobial proper-
ties [11,12]. These disadvantages limit their broad uses,
particularly for the purposes of food packaging. Therefore,
to cater this problem, materials scientists conducted several
studies to enhance the antimicrobial properties without
affecting their biodegradability.
Natural fibres such as cotton [13], rice husk [14,15],
kenaf [16], water hyacinth [17],flax [18], jute [18], ginger
Razali M. O. Syafiq: Laboratory of Biocomposite Technology,
Institute of Tropical Forestry and Forest Products (INTROP),
Universiti Putra Malaysia, 43400 UPM Serdang, Selangor, Malaysia
* Corresponding author: Salit M. Sapuan, Laboratory of
Biocomposite Technology, Institute of Tropical Forestry and Forest
Products (INTROP), Universiti Putra Malaysia, 43400 UPM Serdang,
Selangor, Malaysia; Advanced Engineering Materials and
Composites Research Centre (AEMC), Department of Mechanical
and Manufacturing Engineering, Universiti Putra Malaysia, 43400
UPM Serdang, Selangor, Malaysia, e-mail: sapuan@upm.edu.my
Mohd R. M. Zuhri: Advanced Engineering Materials and Composites
Research Centre (AEMC), Department of Mechanical and
Manufacturing Engineering, Universiti Putra Malaysia, 43400 UPM
Serdang, Selangor, Malaysia
Nanotechnology Reviews 2020; 9: 1147–1159
Open Access. © 2020 Razali M. O. Syafiqet al., published by De Gruyter. This work is licensed under the Creative Commons Attribution 4.0
International License.
[19,20]and sugar palm [21]from plants have attracted the
attention of many researchers in the past, and they are
used because of their important properties such as low
cost of materials, ease of availability and biodegrad-
ability [22]. For example, cotton fibres were used by Boufi
et al. [13]with plasmonic nanoparticles for the destruction
of harmful molecules. Rice husk fibres were also used in the
development of aluminium-based green metal composites
to reduce soil pollution [14].Jainetal.[15]used agricultural
wastericehusk–reinforced epoxy for coating, electronic
implements, aerospace and automotive structures. Besides
that, many scientists have made an effort on cellulose fibre
as conducting composites (i.e. activated carbon)using
binder [22].Thompsonetal.[23]reported research on
cellulose nanocrystals made from woods. The cellulose
crystals were made into composites to produce transparent
films, which have good mechanical properties. Bukit et al.
[24]represented the work on nanoparticles made from oil
palm boiler ash from a palm oil mill. The materials were
characterized by X-ray diffraction (XRD)and Fourier trans-
forms infrared (FTIR), and the materials showed great
potential in nanocomposite industry. Similar work was
represented by Chu et al. [25]on fly ashes and was also
characterized using XRD, FTIR and scanning electron
microscopy (SEM), which showed promising results.
This shows that natural fibre had many advantages to
be used in various applications. In the current research
sugar palm fibres (SPMs)are used as reinforcement in
starch composites in the form of nanocelluloses. One
important advantage of using bio-nanocellulose in com-
positesinfoodpackagingisitsusedoesnotposeany
health hazard unlike nanoparticles made from synthetic
materials [26]. In food packaging, nanocellulose compo-
site had better antibacterial activity than its individual
constituent (starch and fibre)[27].
The natural fibre–reinforced natural polymer had good
advantages over synthetic fibre in terms of biodegrad-
ability, recyclability and low cost per weight to resist tensile
load [28]. Therefore, selection of the right packaging tech-
nologies and materials is a vital aspect in preserving food
freshness and quality as well as reducing environmental
pollutants. One possibility that is being researched exten-
sively is the inclusion of active substances, e.g. essential oil
(EO)in the packaging contents as biopolymer starch-based
films. [29]. To help improving and preserving the food
safety, scientists havedeveloped a novel packaging, known
as active packaging (AP). It might also be a beneficial alter-
native for both conventional and modified packaging, in
terms of preservatives’usage, because it provides microbial
protection to the food by decreasing and inhibiting the
growth of microorganisms, which subsequently extends
the shelf-life of the packed food [30]. Natural antimicro-
bial ingredients have acquired rising demand as custo-
mers are more conscious of possible health hazards as-
sociated with the use of preservatives as well as aware of
the effectiveness of AP [31–34]. Natural ingredients with
antimicrobial activity include lemon oil [35], lemongrass
[36,37], peppermint oil [37–39], cinnamon [29,37,39–42],
lavender [43], Mexican oregano [44], neem [45], tea tree
[39,46],Lavandula angustifolia [47],Mentha pulegium
[47], turmeric [48],lime[49],Origanum vulgare L. [50],
Ziziphora clinopodioides [51], grape seed [51]and Zataria
multiflora Boiss [52].
Sugar palm starch (SPS)is being extensively used in
the manufacturing of bio-based starch films and yielded
promising results [3,21,61,53–60]. SPS films are defined
as non-toxic, colourless, biodegradable, tasteless, odour-
less and isotropic. In a previous study performed by Ilyas
et al. [21], SPS films that were plasticized with glycerol
and sorbitol and reinforced with sugar palm nanocellu-
lose (SPN)were developed [62–65]. The reported findings
were significant as they provided information on an ideal
formulation to manufacture composite film with enhanced
mechanical, thermal and water barrier characteristics. There-
fore, authors are currently attempting to incorporate the SPS
films’formulation with antimicrobial agents as the carrier of
natural additives that might in the foreseeable future be seen
as new tendencies in the functional food packaging. AP pro-
vides the customer with microbial protection by reducing or
inhibiting the growth of microorganisms, which could then
prolong the shelf-life of the food.
A research conducted by Kechichian et al. [66]on
cassava starch had incorporated clove and cinnamon es-
sential oils (CEOs)and showed reduction in tensile proper-
ties, whereas water vapour permeability showed increment
compared to control. These EOs were chosen as raw mate-
rials in the continuation of their research, which was per-
formed by the same researchers as the present study. Besides
that, other authors who presented antimicrobial effective-
ness of cinnamon agents in literature include Souza et al.
[29], Iamareerat et al. [40],Utamietal.[41],Liakosetal.[39],
Rojas-Graü et al. [37]and Nazari et al. [42].Themaincon-
stituent of cinnamon oils is cinnamaldehyde, a well-known
agent because of its antimicrobial activities.
EOs are plant based having volatile, natural and com-
plexcompounds.Besideshavingstrongodour,theybecome
interesting additives in food industry for having good med-
icinal and antimicrobial properties, as well as providing
health benefits. EOs are dissolved with a surfactant because
it is insoluble in water (hydrophobic). Tween 80 and Span
80 are two commonly used surfactants in hydrophile–
lipophile balance [67]. Cinnamon was mainly used as spice
1148 Razali M. O. Syafiqet al.
for a long time, which contains main constituents like
cinnamaldehyde and eugenol that are two important agents
in antimicrobial activities [68]. Cinnamon EOs were reported
to have good antimicrobial activity against meat-isolated
Pseudomonas putida strain [30]. It was also reported that
they had high activity on preventing the spoilage of fungi
on bread. Oussalah et al. [69]revealed that cinnamon EOs
were among the most active EOs, as screened for four patho-
genic bacteria. In the current research, SPS films were devel-
oped via solution casting technique and were incorporated
with cinnamon EOs.
None of the preceding studies, based on a literature
survey, has discussed the effects of CEO on the flamm-
ability and thermal stability as well as morphology of
biopolymer composites of SPN reinforced with SPS. It is
well known in composites that the use of nanofillers such
as nanocelluloses is important in influencing the compo-
site properties such as thermal performances [70]. Lapčík
et al. [70]reported that nanofillers are commonly used for
structural and non-structural components, and packa-
ging as well as advanced coating applications. Therefore,
this study aimed to investigate the possible effects of
using EO as fillers on the flammability, thermal stability
and morphological properties of SPN/SPS biopolymer
composites at different loadings.
2 Materials and methods
2.1 Materials
There are several places in Malaysia that are planted with
sugar palm, hence becoming the sources for SPS and SPF.
In this study, SPF and SPS were obtained from a village in
Kuala Jempol, Negeri Sembilan, Malaysia. Chemicals used,
e.g. sodium hydroxide (NaOH),ethanoicacid(CH
3
COOH),
Sodium chlorite (NaClO
2
), sorbitol, glycerol and Tween 80,
were purchased from Sue Evergreen Sdn. Bhd., Semenyih,
Selangor, Malaysia.
2.2 SPS extraction and preparation
SPS was removed from inside the stem of a matured sugar
palm tree using a chainsaw. The starch powder then
underwent washing process by adding water to the mix-
ture and followed by using a special designed extractor
machine for sugar palm to extract the starch from the
mixture. The mixture was then filtered using a sieve
(<300
µ
m), where the fibre remained at the top of the
sieve and starch granules flowed with the water into
the container. The starch was separated from the water
by pouring the water slowly until it reached the level of
the starch as it is denser than water. Fibre residues that
are by-products were isolated from wet starch. Then, the
wet starch was sun dried for 30 min and oven dried at
120°C for 24 h [71].
2.3 SPF extraction and preparation
SPF is located on the stem of sugar palm tree as natural
woven shape fibre. SPF wraps up the tree trunk and
worker used an axe to cut and remove it from the tree.
Then SPF was ground and filtered to 2 mm size.
2.4 Cellulose extraction
The two main processes carried out to extract the cellulose
fibres from the SPF were delignification and mercerization.
Lignin was removed from SPF to get the holocellulose
through chlorination and bleaching processes according
to ASTM D1104-56 (1978). According to ASTM D1103-60
(1977),α-cellulose is produced through further treatment
of holocellulose [72].
2.5 Separation of sugar palm
nanocrystalline celluloses
Acid hydrolysis method was used to prepare sugar palm
nanocrystalline celluloses (SPNCCs). Cellulose was mixed
with the aqueous H
2
SO
4
(60 wt%)at 5:100 ratio (wt%)and
was stirred at 45°C for 45 min at a rotation speed of
1,200 rpm using a mechanical stirrer. Then, washing pro-
cess took place for the hydrolysed cellulose for four repeti-
tions through centrifugation (6,000 rpm, 20 min and 20°C)
to remove all the leftover H
2
SO
4
. Next, the cellulose was
dialysed using distilled water until neutral pH (6.5–7)was
reached. Sonication process was performed to the cellulose
using a sonicator for 30min. The final cellulose was freeze
dried and kept in cool place before further analysis and
application as starch film’sreinforcement.
Effect of CEO on starch biopolymer composites 1149
2.6 Preparation of SPS/SPNCCs-
incorporated CEO nanocomposite films
Composite films from SPNCCs were prepared by solution
casting technique. Firstly, all materials and solutions
such as sorbitol, glycerol, starch (10 g),SPNCCs(0.05 g),
cinnamon EOs, tween 80 and distilled water (190 mL)were
prepared. All the solutions were mixed together by simple
stirring, and the mixture was put into the sonicator to pro-
duce a homogenous nanocomposite film. About 190 mL of
distilled water was added to the prepared solution with
different concentrations of cinnamon EOs, as presented in
Table 1, and the solutions were sonicated for 30 min. After
sonication process, 10 g of SPS solution was poured and
stirredfor20minat1,000rpmat85°Cinadisperserto
gelatinize the starch. This process is vital to assure that
homogenous dispersion happened simultaneously and the
starch granules were uniformly degraded. The ratio of plas-
ticizers used was 1:1, which was about 1.5 wt% of the
plasticizers in this experiment. The film-forming process
was performed under vacuum condition so that the air
bubbles were removed. Then, the solution-casting process
was performed by pouring 45 g of the suspension into a
15 cm diameter petri dish. The setup was then kept in
an oven for overnight drying at 40°C. Next, the film was
removed from the petri dish and kept in a controlled room
at 23 ±2°C and relative humidity of 53 ±1% for 7 days.
2.7 Scanning electron microscopy
Afieldemissionelectronmicroscope(FEI NOVA NanoSEM
230, Czech Republic)was used to investigate the morphology
of the films. All the samples were gold-coated by using
aplasmaargon(sputter coater K575X; Edwards Limited,
Crawley, United Kingdom)to prevent unwanted charging.
The SEM testing was conducted at a 3 kV acceleration
voltage.
2.8 Thermogravimetric analysis
The thermal stability of the samples was investigated using
a Q series thermal analysis machine (TA Instruments, New
Castle, DE, USA). The process was conducted in an alumi-
nium vessel in dynamic nitrogen environment. The heating
rate was fixedat10°C/mintoheatthesamplesinatem-
perature range of 25–800°C. About 5–15 mg of the sample
was put in the metallic vessel and was made ready for the
heating process. Then, the temperature was increased for
strong heating. The weight loss determination was analysed
from the plot of per cent of mass loss against temperature
(thermogravimetric analysis [TGA]curve).
2.9 Flammability test
Flammability test was carried out for all samples via hor-
izontal burning test according to ASTM D635 with slight
modification. Samples having dimensions of 120 mm ×
10 mm ×0.2 mm were prepared and two lines at 25 and
100 mm from one end of the sample were drawn as the
reference marks. Then, fire was ignited with natural gas
on one end of the sample. The overall burnt length and
the time taken for the flame to spread to the 25 and
100 mm reference marks were noted. The linear rate of
the burning samples was calculated using equation (1).
=/VLt60 ,
(1)
where Vis the linear burning rate (mm/min),Lis the
burnt length (mm)and tis the time (minutes).
3 Results and discussion
3.1 Microscopy analysis
SPS-based films that are homogeneous, flexible and thin
(0.25 mm)were obtained. After drying, they were easily
peeled offthe petri dish plates. From the observation,
all films were yellowish in colour and slightly opaque
(Figure 1). The microstructure test was performed to
determine the appearance and presence of EO on the
morphological surface of the biofilms. Microscopic film
analysis is closely linked to the physical properties of the
final materials of biofilms, including the visual, mechan-
ical and barrier properties. Figure 2 displays the scanning
electron microscopy (SEM)micrographs corresponding
Table 1: Denotations of SPS/SPNCC-incorporated CEO nanocom-
posite films
Denotation of
the films
Formulation
Sorbitol
(wt%)
Glycerol
(wt%)
CEO
(wt%)
1 1.5 1.5 0
2 1.5 1.5 0.8
3 1.5 1.5 1.2
4 1.5 1.5 1.6
5 1.5 1.5 2.0
1150 Razali M. O. Syafiqet al.
to the biofilm surfaces and also the SEM micrographs of
active SPS films surface with remarkable changes. The
control film surface without CEO exhibited a smooth
and uniform texture without traces of starch granular or
cracks (Figure 2a). The finding is similar to Ilyas et al.
[21,53,60]who also reported the appearance of contin-
uous and smooth microstructure for SPS film. Meanwhile,
Acosta et al. [73], who studied the microstructure of starch–
gelatin (SG)blend films, revealed that neat SG composite
films (without EO)showed heterogeneous structures on
their surface. Formation of circles was detected on the sur-
face of the SG films because of the incomplete miscibility of
starch and gelatin. It was also associated with the polymer
separation phase that gave rise to starch-rich phase that
was interpenetrated with a gelatin-rich phase. The incor-
poration of CEO in SPN/SPS biofilms affected the SPS matrix
microstructure, as presented in Figure 2b–e. Adding 0.8, 1.2,
1.6% and 2.0% CEO to the SPN/SPS biofilm yielded uneven
surface structures with the increasing surface coarseness
with CEO concentration (Figure 2b–f), similar to the findings
reported by Choi et al. [74]. Since the surface of the pure film
had no micro-porous holes, these phenomena may be
caused by the evaporation of essential oils after the drying
process [29].InFigure2b–f, irregularities were exhibited in
cross-section images of the control film that looked like a
network of fibres. Homogenous and smooth surface was
observed in Figure 2a, without the presence of micro-
porous holes. The formation of this microstructure might
be associated with the incomplete dissolution/gelatiniza-
tion of starch granules that are held together by the
solubilized-gelatinized starch fraction [29]. Similar re-
sults were obtained for different starch-based films as
reported in ref. [4,29,43]and other authors. The crosssec-
tion of the films revealed the micro-porous spots that
emerged as micro-porous holes under the micrographs
(Figure 2b–e). The number and size of the microporous
holes were found to increase with concentrations of CEO.
The appearance of abundant holes corresponded to the po-
sition of the oil droplets, where these droplets could
partially vaporize on the cryo-fractured surface during
SEM analysis because of the high vacuum condition. They
were elongated, which, as previously noted, could be ex-
plained by their distortion during drying of the film and
consecutive packaging of the polymer chains [29]. Similar
results were obtained by Peng and Li [75]and Sánchez-
González et al. [76], who worked with lion oil and tea tree
EO that were added to chitosan films and hydroxypropyl
methylcellulose films, respectively.
3.2 FTIR spectroscopy analysis
The FTIR spectra of the control SPS/SPNCC nanocomposite
film and SPS/SPNCC nanocomposite films incorporated with
various concentration of cinnamon EO are shown in Figure 3.
The purpose of this analysis was to identify the changes
occurred in the chemical structures of the films. Intermole-
cular rearrangement of polysaccharide chain orientation can
be recognized by analysing the spectral differences between
the films. The peak at 996 cm
−1
was associated with C–O
bond of C–O–C groups. The high peak that displayed at
2,926 cm
−1
was assigned to C–H stretching, whereas the
low peak at 1,644 cm
−1
corresponded to C–Ostretching.
O–H group assigned at the broad peak of the film, which
was observed from 3,000 to 3,700 cm
−1
, is an indicator of
hydrophilic properties because of the presence of hydroxyl
group in nanofibre. These findings reflectthoseofIlyasetal.
[77].Thepeakat1,735cm
−1
was associated with aldehyde
groups [78,79]. According to Salzer et al. [78]and Shankara-
narayana et al. [79], CEO contains a high amount of
aldehyde. An absorbance peak at 1,733 cm
−1
appeared in
cinnamon EO-incorporated films, and this peak shifted
from 1,733 to 1,735 cm
−1
as the concentration increased [79].
The broad peaks at 3,000–3,500 cm
−1
were because of
the relative peak strength of stretching vibrations for O–H
groups in the films. Films incorporated with cinnamon EO
had higher amplitude of peaks near 3,266 cm
−1
.Thisindi-
cates the presence of EO that contains hydrocarbons in the
matrix. As the EO concentrations in the films increased,
the peak at wavenumber 3,266 cm
−1
shifted to 3,282 cm
−1
.
The peak shifting can be attributed to the fact that hydrogen
bonding between molecules was partially destroyed [62].
Figure 1: Transparent film of CEO-reinforced SPN/SPS biocompo-
site film.
Effect of CEO on starch biopolymer composites 1151
The differences in absorption peaks for films incorporated
with cinnamon EO indicated that the molecular structure
had been altered [80]. It is probably because of the
formation of hydrogen bonding between hydroxyl group
and cinnamon EO compounds. The peak shifting from
lower to higher wavenumber was largely attributed to
Figure 2: SPN/SPS biocomposite film incorporated with (a)0%, (b)0.8%, (c)1.2%, (d)1.6 and (e)2.0% of CEO.
1152 Razali M. O. Syafiqet al.
different conformations of molecular structures induced
by the addition of cinnamon EO.
Furthermore, the peak at 996 cm
−1
was shifted to
997 cm
−1
probably because of new interaction between
C–O stretching vibrations for EOs and the starch mole-
cules. The changes in wavenumberwere probablycaused by
theelectronjumpsbetweenorbitalswithwell-defined energy
differences, and the bonds in the given molecules may bend,
rotate or stretch with certain frequencies [81].Theresultalso
showed a similar IR spectrum compared to control film. The
increase in EO concentration caused the inter/intra-mole-
cular interaction existed between the starch and the EO via
hydrogen bonding or the van der walls force [77]. The band
greater than 996 cm
−1
was attributed to C–Ostretchingvibra-
tions of polysaccharide compound of starch and glycerol
[55]. The results suggested that the addition of cinnamon
EO influenced the molecular interaction of polymer chain
in the film matrix [43]. As the substances were mixed, phy-
sical blends against chemical reactions caused changes in
the spectral peak [82]. It is generally known that hydrogen
bonding will increase the wavenumber of bending vibrations
but decrease the wavenumber of stretching vibrations [81].
The FTIR results indicate the existence of the interaction
between SPS and cinnamon EO.
3.3 Thermogravimetric analysis
The effect of the CEO on the thermal stability of the com-
posites was examined by TGA and derivative thermo-
gravimetry (DTG)curves, and the results are presented
in Figure 4. Thermal analysis test allows food manufac-
turers to optimize production, storage, transportation,
cooking and consumption quality of the food. TGA techni-
ques continually examined the mass of a sample as it is
heated or cooled at a regulated rate or is held at a selected
temperature for a set length of time. TGA is useful for
tracking processes that involve a shift in the mass of a
food packaging materials, and applications typically in-
volve evaporation, desorption and vaporization behaviour,
as well as thermal stability, decomposition and composi-
tional investigation. Besides that, the TGA indicates max-
imum temperature for the food packaging to package food.
From the thermograms, it can be observed that both the SPN/
SPS and the CEO/SPN/SPS biocomposite films degraded in
similar steps, as shown in Figure 4. In the TGA and DTG
curves of control SPS, multi-step thermal decomposition
events have been observed. Similar results with two-step
thermal decompositions in majority of starch-based films
were obtained and reported in the literatures [21,54].Apart
from that, the mass loss of the sample was decreased with
the increment of CEO loading, as stated in Table 2. The first
degradation step represented by small peak DTG curve
occurred below 100°C, approximately at T
max
≈69–90°C.
This was because of the evaporation of the broken inter-
and intra-molecular hydrogen bonds followed by loss of
water. Besides that, mass loss at this temperature range
might also be because of the removal of water or evaporation
of low molecular weight compounds and loosely bonded
waterinthesample.AsmoreCEOaddedinthefilm solution,
the amount of water decreased. The same phenomenon was
observed to occur for the other film samples, including con-
trol SPS, as can be clearly seen in their DTG curves.
A prolonged pyrolysis process took place at 200–370°C
and reached maximum mass loss at 296.25°C. From Figure
4, it was obvious that control film was less stable compared
to other films, having the lowest decomposition tempera-
ture of 289°C compared to CEO-reinforced SPN/SPS bio-
composites. The weight loss might be associated with the
vaporization and decomposition (oxidative and thermal)of
bio-polymers and elimination of glycerol and volatile pro-
ducts [54,83]. In the TGA thermogram of CEO/SPN/SPS, the
weight loss was initiated at around 40°C, showing an onset
point at around 80°C, indicating that CEO has volatile
nature. The flash point of cinnamon oils is between 38
and 60°C.
The thermal stability of polymer networks was shown
to be improved by the CEO, as control films displayed lower
weight loss temperature (T
max
≈289.18°C)than CEO films.
The thermal stability of the films increased with the loading
of CEO. The lowest loading (CEO sample 1)resulted in
lower thermal stability and was increased with increased
Figure 3: FTIR spectra of cinnamon EO-incorporated SPS/SPNCC
nanocomposite films.
Effect of CEO on starch biopolymer composites 1153
loading (CEO samples 2 and 3). This phenomenon could be
associated with polymer structure rearrangement fol-
lowing the addition of higher CEO concentrations. It was
observed that the polymer structure changed with the smal-
lest quantity of CEO, but upon adding more CEO, the thermal
stability increased. This was related to the rise in crystallinity
indexes when the CEO concentration increased, as described
by Noshirvani et al. [84].Maetal.[85],whoobservedthe
same pattern, concluded that the use of olive oil in the film
matrix has led to an increased gelatine transition helix–coil
temperature. They decided that olive oil created non-mis-
cible emulsified phases in the films. The thermal stability
is also parallel to the degree of crystallinity. Higher degree
of crystallinity resulted in higher thermal stability [21,54,86].
This was ascribed to lower neat SPS values similar to the
findings also observed in other works [87,88].
Figure 4: TGA and DTG curves of SPN/SPS and CEO/SPN/SPS biocomposite films in different concentrations.
1154 Razali M. O. Syafiqet al.
3.4 Flammability analysis
Plastics have become one of the most useful materials
known to humankind. Because of their chemical composi-
tion, plastics can easily ignite when exposed to sufficient
heat in the presence of oxygen. Because of the rate of
burning for plastics, considerable work has been directed
to study and minimize the flammability issues of these
materials, like the addition of flame retardant chemicals
to prevent or minimize the combustion of these materials.
This test is done to classify and measure burning charac-
teristics of plastics. Figure 5 shows the effect of varying
CEO loadings on the flammability of SPN/SPS com-
posites, as indicated by the linear burning rate. The
burning rate was increased with CEO concentration.
With 2% CEO, the SPN/SPS biocomposite displayed the
shortest burnout time compared to the unfilled compo-
sites and then had the highest linear burning rate. Most
EOs, including CEO, are extremely flammable [89–91].
CEO possesses complex mixture comprising over 300
different compounds [92,93]. CEO consists of volatile
organic compounds, typically having molecular weight
below 300 [94,95]. The volatile compounds are from
different chemical classes, such as ethers and oxide,
ketones, alcohols, amines, aldehydes, phenols, esters
and amides. The flash point for CEO is 71°C, which ex-
plained the flammability characteristic of the film com-
posites. During the burning process, the CEO formed a
non-protective oil layer on the surface of the matrix,
serving as an oxygen conductor and permitting heat to
penetrate the matrix [96,97]. Therefore, the quantity of
decomposed volatiles that escaped the interior polymer
matrix was increased, resulting in a shorter burning
time and thus increasing the linear burning rate.
4 Conclusions
The thermal stability of the CEO/SPN/SPS biopolymer
composites was remarkably improved with increasing
CEO loadings (sample 5, T
max
=296.25°C)compared to
the thermal stability of the unfilled compound (sample 1,
T
max
=289.18°C). The control film surface without CEO
displayed a uniform and smooth texture with no traces of
starchgranularorcrack.ThepresenceoftheCEOinthe
SPN/SPS biofilms affected the microstructures of the SPS
matrix, resulting in rough surface structures and increased
surface coarseness with CEO concentrations. The appear-
ance of numerous holes was consistent with the position of
oil droplets, where the number of holes rose as EO loading
increased. Because of the high vacuum situation, this can
partially evaporate on the cryo-fractured surface during
SEM study. The linear burning rate was increased with
the CEO concentration. The SPN/SPS biocomposite with
2% CEO showed the shortest burnout time compared to
the unfilled composites and hence had the fastest linear
burning rate.
Acknowledgements: TheauthorsarethankfultoUniversiti
Putra Malaysia (UPM)for the financial support via the
Graduate Research Assistantship (GRA), Ministry of Higher
Education Malaysia Grant scheme HiCOE (6369107),
Fundamental Research Grant Scheme (FRGS): FRGS/1/
2017/TK05/UPM/01/1 (5540048)and Geran Putra Berim-
pak (GPB), UPM/800-3/3/1/GPB/2019/9679800.
Conflict of interest: The authors declare no conflict of
interest regarding the publication of this paper.
References
[1]Ilyas RA, Sapuan SM, Kadier A, Kalil MS, Ibrahim R,
Atikah MSN, et al. Properties and characterization of PLA, PHA,
and other types of biopolymer composites. In: Al-Oqla F,
Sapuan SM, editors. Advanced Processing, Properties, and
Applications of Starch and Other Bio-Based Polymers. 1st ed
Elsevier; 2020. p. 111–38.
[2]Lee CH, Sapuan SM, Ilyas RA, Lee SH, Khalina A. Development
and processing of PLA, PHA, and other biopolymers. In: Al-
Oqla F, Sapuan SM, editors. Advanced processing, properties,
and applications of starch and other bio-based polymers. 1st
ed Elsevier; 2020. p. 47–63.
[3]Sanyang ML, Ilyas RA, Sapuan SM, Jumaidin R. Sugar palm
starch-based composites for packaging applications.
Bionanocomposites for Packaging Applications [Internet].
Cham: Springer International Publishing; 2018. p. 125–47.
0
100
200
300
400
500
600
700
Control 0.8 1.2 1.6 2
Rate of burning (mm/min)
CEO loading (%)
Figure 5: The effect of different CEO loadings on the flammability of
SPN/SPS biocomposite film.
Effect of CEO on starch biopolymer composites 1155
Available from: http://link.springer.com/10.1007/978-3-319-
67319-6_7.
[4]Song X, Zuo G, Chen F. Effect of essential oil and surfactant on
the physical and antimicrobial properties of corn and wheat
starch films. Int J Biol Macromol [Internet]. 2018
Feb;107:1302–9. Available from: https://linkinghub.else-
vier.com/retrieve/pii/S0141813017320378.
[5]Ilyas RA, Sapuan SM. Biopolymers and biocomposites:
Chemistry and technology. Curr Anal Chem. 2020
Jul;16(5):500–3.
[6]Ilyas RA, Sapuan SM. The preparation methods and processing
of natural fibre bio-polymer composites. Curr Org Synth. 2020
Jan;16(8):1068–70.
[7]Ilyas RA, Sapuan SM, Sanyang ML, Ishak MR, Zainudin ES.
Nanocrystalline cellulose as reinforcement for polymeric ma-
trix nanocomposites and its potential applications: A review.
Curr Anal Chem [Internet]. 2018 May 7;14(3):203–25. Available
from: http://www.eurekaselect.com/156148/article.
[8]Ayu RS, Khalina A, Harmaen AS, Zaman K, Isma T, Liu Q, et al.
Characterization study of empty fruit bunch (EFB)fibers rein-
forcement in poly(Butylene)succinate (PBS)/starch/glycerol
composite sheet. Polymers. 2020 Jul;12(7):1571.
[9]Jumaidin R, Khiruddin MAA, Asyul Sutan Saidi Z, Salit MS,
Ilyas RA. Effect of cogon grass fibre on the thermal, mechanical
and biodegradation properties of thermoplastic cassava
starch biocomposite. Int J Biol Macromol. 2019;146:746–55.
[10]Abral H, Basri A, Muhammad F, Fernando Y, Hafizulhaq F,
Mahardika M, et al. A simple method for improving the prop-
erties of the sago starch films prepared by using ultrasonica-
tion treatment. Food Hydrocoll. 2019 Aug;93:276–83.
[11]do Evangelho JA, da Silva Dannenberg G, Biduski B, el
Halal SLM, Kringel DH, Gularte MA, et al. Antibacterial activity,
optical, mechanical, and barrier properties of corn starch films
containing orange essential oil. Carbohydr Polym. 2019
Oct;222:114981.
[12]Pirouzifard M, Yorghanlu RA, Pirsa S. Production of active film
based on potato starch containing Zedo gum and essential oil
of Salvia officinalis and study of physical, mechanical, and
antioxidant properties. J Thermoplast Compos Mater.
2020;33(7):915–37.
[13]BoufiS, Bouattour S, Ferraria AM, Ferreira LFV, Rego AMB D,
Chehimi MM, et al. Cotton fibres functionalized with plasmonic
nanoparticles to promote the destruction of harmful
molecules: An overview. Nanotechnol Rev. 2020;8(1):
671–80.
[14]Dwivedi SP, Dwivedi G. Utilization of RHA in development of
hybrid composite by electromagnetic stir casting technique
using RSM. J Mech Behav Mater. 2019;29(4):45–54.
[15]Jain N, Somvanshi KS, Gope PC, Singh VK. Mechanical char-
acterization and machining performance evaluation of rice
husk/epoxy an agricultural waste based composite material.
J Mech Behav Mater. 2019;28(1):29–38.
[16]Mazani N, Sapuan SM, Sanyang ML, Atiqah A, Ilyas RA. Design
and fabrication of a shoe shelf from kenaf fiber reinforced
unsaturated polyester composites. Lignocellulose for Future
Bioeconomy. Elsevier; 2019. p. 315–32.
[17]Syafri E, Mashadi S, Yulianti E, Mochamad AsrofiD, Abral H,
Sapuan SM, et al. Effect of sonication time on the thermal
stability, moisture absorption, and biodegradation of water
hyacinth (Eichhornia crassipes)nanocellulose-filled
bengkuang (Pachyrhizus erosus)starch biocomposites. J
Mater Res Technol. 2019 Nov;8(6):6223–31.
[18]Chen C, Yang Y, Zhou Y, Xue C, Chen X, Wu H, et al.
Comparative analysis of natural fiber reinforced polymer and
carbon fiber reinforced polymer in strengthening of reinforced
concrete beams. J Clean Prod [Internet]. 2020;263:121572.
Available from: https://doi.org/10.1016/
j.jclepro.2020.121572.
[19]Abral H, Ariksa J, Mahardika M, Handayani D, Aminah I,
Sandrawati N, et al. Highly transparent and antimicrobial PVA
based bionanocomposites reinforced by ginger nanofiber.
Polym Test. 2019 Oct;(October):106186.
[20]Abral H, Ariksa J, Mahardika M, Handayani D, Aminah I,
Sandrawati N, et al. Transparent and antimicrobial cellulose
film from ginger nanofiber. Food Hydrocoll. 2020
Jan;98:105266.
[21]Ilyas RA, Sapuan SM, Ishak MR, Zainudin ES. Development and
characterization of sugar palm nanocrystalline cellulose rein-
forced sugar palm starch bionanocomposites. Carbohydr
Polym. 2018;202:186–202.
[22]Ventrapragada LK, Creager SE, Rao AM, Podila R. Carbon na-
notubes coated paper as current collectors for secondary li-ion
batteries. Nanotechnol Rev. 2019;8(1):18–23.
[23]Thompson L, Azadmanjiri J, Nikzad M, Sbarski I, Wang J, Yu A.
Cellulose nanocrystals: Production, functionalization and ad-
vanced applications. Rev Adv Mater Sci. 2019;58(1):1–16.
[24]Bukit N, Ginting EM, Hutagalung EA, Sidebang E, Frida E,
Bukit BF. Preparation and characterization of oil palm ash from
boiler to nanoparticle. Rev Adv Mater Sci. 2019;58(1):195–200.
[25]Chu YS, Davaabal B, Kim DS, Seo SK, Kim Y, Ruescher C, et al.
Reactivity of fly ashes milled in different milling devices. Rev
Adv Mater Sci. 2019;58(1):179–88.
[26]Naseer B, Srivastava G, Qadri OS, Faridi SA, Islam RU,
Younis K. Importance and health hazards of nanoparticles
used in the food industry. Nanotechnol Rev.
2018;7(6):623–41.
[27]Das S, Srivastava VC. An overview of the synthesis of CuO-ZnO
nanocomposite for environmental and other applications.
Nanotechnol Rev. 2018;7(3):267–82.
[28]Chen C, Yang Y, Yu J, Yu J, Tan H, Sui L, et al. Eco-friendly and
mechanically reliable alternative to synthetic FRP in externally
bonded strengthening of RC beams: Natural FRP. Compos
Struct [Internet]. 2020;241(February):112081. Available from:
https://doi.org/10.1016/j.compstruct.2020.112081.
[29]Souza AC, Goto GEO, Mainardi JA, Coelho ACV, Tadini CC.
Cassava starch composite films incorporated with cinnamon
essential oil: Antimicrobial activity, microstructure, mechan-
ical and barrier properties. LWT -Food Sci Technol [Internet].
2013 Dec;54(2):346–52. Available from: https://linkinghu-
b.elsevier.com/retrieve/pii/S002364381300234X.
[30]Nielsen PV, Rios R. Inhibition of fungal growth on bread by
volatile components from spices and herbs, and the possible
application in active packaging, with special emphasis on
mustard essential oil. Int J Food Microbiol.
2000;60(2–3):219–29.
[31]Ju J, Chen X, Xie Y, Yu H, Guo Y, Cheng Y, et al. Application of
essential oil as a sustained release preparation in food
packaging. Trends Food Sci Technol. 2019 Oct;92:22–32.
[32]Bhavaniramya S, Vishnupriya S, Al-Aboody MS,
Vijayakumar R, Baskaran D. Role of essential oils in food
1156 Razali M. O. Syafiqet al.
safety: Antimicrobial and antioxidant applications. Grain Oil.
Sci Technol. 2019;49–55.
[33]Atarés L, Chiralt A. Essential oils as additives in biodegradable
films and coatings for active food packaging. Trends Food Sci
Technol. 2016;48:51–62.
[34]Donsì F, Ferrari G. Essential oil nanoemulsions as antimicro-
bial agents in food. J Biotechnol. 2016;233:106–20.
[35]Song X, Zuo G, Chen F. Effect of essential oil and surfactant on
the physical and antimicrobial properties of corn and wheat
starch films. Int J Biol Macromol. 2018;107(PartA):1302–9.
[36]Resianingrum R, Atmaka W, Khasanah LU, Kawiji, Utami RPD.
Characterization of cassava starch-based edible film enriched
with lemongrass oil (Cymbopogon citratus). Nusant Biosci
[Internet]. 2016 Dec 1;8(2):278–82. Available from: http://
biosains.mipa.uns.ac.id/N/N0802/N080223.pdf.
[37]Rojas-Graü MA, Avena-Bustillos RJ, Olsen C, Friedman M,
Henika PR, Martín-Belloso O, et al. Effects of plant essential
oils and oil compounds on mechanical, barrier and antimi-
crobial properties of alginate-apple puree edible films. J Food
Eng. 2007;81(3):634–41.
[38]Liang R, Xu S, Shoemaker CF, Li Y, Zhong F, Huang Q. Physical
and antimicrobial properties of peppermint oil nanoemul-
sions. J Agric Food Chem. 2012;60:7548–55.
[39]Liakos I, Rizzello L, Scurr DJ, Pompa PP, Bayer IS,
Athanassiou A. All-natural composite wound dressing films of
essential oils encapsulated in sodium alginate with antimi-
crobial properties. Int J Pharm [Internet]. 2014;463(2):137–45.
Available from: http://dx.doi.org/10.1016/
j.ijpharm.2013.10.046.
[40]Iamareerat B, Singh M, Sadiq MB, Anal AK. Reinforced cassava
starch based edible film incorporated with essential oil and
sodium bentonite nanoclay as food packaging material. J Food
Sci Technol [Internet]. 2018 May 5;55(5):1953–9. Available
from: http://link.springer.com/10.1007/s13197-018-3100-7.
[41]Utami R, Khasanah LU, Manuhara GJ, Ayuningrum ZK. Effects of
cinnamon bark essential oil (cinnamomum burmannii)on
characteristics of edible film and quality of fresh beef.
Pertanika J Trop Agric Sci. 2019;42(4):1173–84.
[42]Nazari M, Majdi H, Milani M, Abbaspour-Ravasjani S,
Hamishehkar H, Lim LT. Cinnamon nanophytosomes em-
bedded electrospun nanofiber: Its effects on microbial quality
and shelf-life of shrimp as a novel packaging. Food Packag
Shelf. Life [Internet]. 2019;21(June):100349. Available from:
https://doi.org/10.1016/j.fpsl.2019.100349.
[43]Jamróz E, Juszczak L, Kucharek M. Investigation of the physical
properties, antioxidant and antimicrobial activity of ternary
potato starch-furcellaran-gelatin films incorporated with la-
vender essential oil. Int J Biol Macromol [Internet].
2018;114(2017):1094–101. Available from: https://doi.org/
10.1016/j.ijbiomac.2018.04.014.
[44]Avila-Sosa R, Hernández-Zamoran E, López-Mendoza I,
Palou E, Munguía MTJ, Nevárez-Moorillón GV, et al. Fungal
inactivation by Mexican oregano (lippia berlandieri schauer)
essential oil added to amaranth, chitosan, or starch edible
films. J Food Sci [Internet]. 2010 Apr;75:M127–33. Available
from: http://doi.wiley.com/10.1111/j.1750-
3841.2010.01524.x3.
[45]Cano A, Cháfer M, Chiralt A. González-Martínez C. Physical and
antimicrobial properties of starch-PVA blend films as affected
by the incorporation of natural antimicrobial agents. Foods
[Internet]. 2015;5(1):3. Available from: http://www.mdpi.com/
2304-8158/5/1/3.
[46]Silveira MP, Silva HC, Pimentel IC, Poitevin CG, da Costa
Stuart AK, Carpiné D, et al. Development of active cassava
starch cellulose nanofiber-based films incorporated with nat-
ural antimicrobial tea tree essential oil. J Appl Polym Sci.
2020;137(21):1–11.
[47]Aitboulahsen M, El Galiou O, Laglaoui A, Bakkali M,
Hassani, Zerrouk M. Effect of plasticizer type and essential oils
on mechanical, physicochemical, and antimicrobial charac-
teristics of gelatin, starch, and pectin-based films. J Food
Process Preserv. 2020;44(6):1–10.
[48]Mustapha FA, Jai J, Nik Raikhan NH, Sharif ZIM, Yusof NM.
Response surface methodology analysis towards biodegrad-
ability and antimicrobial activity of biopolymer film containing
turmeric oil against Aspergillus niger. Food Control [Internet].
2019;99(December 2018):106–13. Available from: https://
doi.org/10.1016/j.foodcont.2018.12.042.
[49]Sánchez Aldana D, Andrade-Ochoa S, Aguilar CN, Contreras-
Esquivel JC, Nevárez-Moorillón GV. Antibacterial activity of
pectic-based edible films incorporated with Mexican lime es-
sential oil. Food Control [Internet]. 2015;50:907–12. Available
from: http://dx.doi.org/10.1016/j.foodcont.2014.10.044.
[50]Hosseini SF, Rezaei M, Zandi M, Farahmandghavi F.
Development of bioactive fish gelatin/chitosan nanoparticles
composite films with antimicrobial properties. Food Chem
[Internet]. 2016;194:1266–74. Available from: http://
dx.doi.org/10.1016/j.foodchem.2015.09.004.
[51]Shahbazi Y. The properties of chitosan and gelatin films in-
corporated with ethanolic red grape seed extract and
Ziziphora clinopodioides essential oil as biodegradable ma-
terials for active food packaging. Int J Biol Macromol [Internet].
2017;99:746–53. Available from: http://dx.doi.org/10.1016/
j.ijbiomac.2017.03.065.
[52]Dashipour A, Razavilar V, Hosseini H, Shojaee-Aliabadi S,
German JB, Ghanati K, et al. Antioxidant and antimicrobial
carboxymethyl cellulose films containing Zataria multiflora
essential oil. Int J Biol Macromol [Internet]. 2015;72:606–13.
Available from: http://dx.doi.org/10.1016/
j.ijbiomac.2014.09.006.
[53]Ilyas RA, Sapuan SM, Ibrahim R, Abral H, Ishak MR,
Zainudin ES, et al. Effect of sugar palm nanofibrillated cellu-
lose concentrations on morphological, mechanical and phy-
sical properties of biodegradable films based on agro-waste
sugar palm (Arenga pinnata (Wurmb.)Merr)starch. J Mater Res
Technol [Internet]. 2019 Sep;8(5):4819–30. Available from:
https://linkinghub.elsevier.com/retrieve/pii/
S2238785419308828.
[54]Ilyas RA, Sapuan SM, Ibrahim R, Abral H, Ishak MR,
Zainudin ES, et al. Thermal, biodegradability and water barrier
properties of bio-nanocomposites based on plasticised sugar
palm starch and nanofibrillated celluloses from sugar palm
fibres. J Biobased Mater Bioenergy. 2020;14:1–13.
[55]Ilyas RA, Sapuan SM, Ibrahim R, Abral H, Ishak MR,
Zainudin ES, et al. Effect of sugar palm nanofibrillated cellu-
lose concentrations on morphological, mechanical and phy-
sical properties of biodegradable films based on agro-waste
sugar palm (Arenga pinnata(Wurmb.)Merr)starch. J Mater Res
Technol [Internet]. 2019;8(5):4819–30. Available from:
https://doi.org/10.1016/j.jmrt.2019.08.028.
Effect of CEO on starch biopolymer composites 1157
[56]Ilyas RA, Sapuan SM, Ishak MR, Zainudin ES, Atikah MSN.
Characterization of sugar palm nanocellulose and its potential
for reinforcement with a starch-based composite. Sugar Palm
Biofibers, Biopolymers, & Biocomposites. 1st ed. Boca Raton:
CRC Press/Taylor & Francis Group; 2018. p. 190–212.
[57]Ilyas RA, Sapuan SM, Kadier A, Krishnan S, Atikah MSN,
Ibrahim R, et al. Mechanical testing of sugar palm fiber rein-
forced sugar palm biopolymer composites. In: Al-Oqla F,
Sapuan SM, editors. Advanced processing, properties, and
applications of starch and other bio-based polymers. 1st ed.
Elsevier; 2020. p. 89–110.
[58]Hazrol MD, Sapuan SM, Ilyas RA, Othman ML, Sherwani SFK.
Electrical properties of sugar palm nanocrystalline cellulose
reinforced sugar palm starch nanocomposites. Polimery. 2020
May;65(5):363–70.
[59]Ilyas RA, Sapuan SM, Atiqah A, Ibrahim R, Abral H, Ishak MR,
et al. Sugar palm (Arenga pinnata [Wurmb.]Merr)starch films
containing sugar palm nanofibrillated cellulose as reinforce-
ment: Water barrier properties. Polym Compos. 2020
Feb;41(2):459–67.
[60]Atikah MSN, Ilyas RA, Sapuan SM, Ishak MR, Zainudin ES,
Ibrahim R, et al. Degradation and physical properties of sugar
palm starch/sugar palm nanofibrillated cellulose bionano-
composite. Polimery. 2019;64(10):27–36.
[61]Ilyas RA, Sapuan SM, Ishak MR, Zainudin ES. Water transport
properties of bio-nanocomposites reinforced by sugar palm
(Arenga Pinnata)nanofibrillated cellulose. J Adv Res Fluid
Mech Therm Sci J. 2018;51(2):234–46.
[62]Ilyas RA, Sapuan SM, Ishak MR. Isolation and characterization
of nanocrystalline cellulose from sugar palm fibres (Arenga
Pinnata). Carbohydr Polym. 2018;181(November
2017):1038–51.
[63]Ilyas RA, Sapuan SM, Ishak MR, Zainudin ES. Sugar palm na-
nofibrillated cellulose (Arenga pinnata (Wurmb.)Merr):Effect
of cycles on their yield, physic-chemical, morphological and
thermal behavior. Int J Biol Macromol [Internet].
2018;123:379–88. Available from: https://linkinghub.else-
vier.com/retrieve/pii/S0141813018331477.
[64]Ilyas RA, Sapuan SM, Ibrahim R, Abral H, Ishak MR,
Zainudin ES, et al. Sugar palm (Arenga pinnata (Wurmb.)Merr)
cellulosic fibre hierarchy: A comprehensive approach from
macro to nano scale. J Mater Res Technol. 2019
May;8(3):2753–66.
[65]Ilyas RA, Sapuan SM, Atikah MSN, Asyraf MRM, Ayu Rafiqah S,
Aisyah HA, et al. Effect of hydrolysis time on the morpholo-
gical, physical, chemical, and thermal behavior of sugar palm
nanocrystalline cellulose (Arenga pinnata (Wurmb.)Merr).
Text Res J. 2020 Jun. 004051752093239.
[66]Kechichian V, Ditchfield C, Veiga-Santos P, Tadini CC. Natural
antimicrobial ingredients incorporated in biodegradable films
based on cassava starch. LWT -Food Sci Technol. 2010
Sep;43(7):1088–94.
[67]Ojagh SM, Rezaei M, Razavi SH, Hosseini SMH. Development
and evaluation of a novel biodegradable film made from chit-
osan and cinnamon essential oil with low affinity toward
water. Food Chem [Internet]. 2010;122(1):161–6. Available
from: http://dx.doi.org/10.1016/j.foodchem.2010.02.033.
[68]Oussalah M, Caillet S, Saucier L, Lacroix M. Antimicrobial
effects of selected plant essential oils on the growth of a
Pseudomonas putida strain isolated from meat. Meat Sci.
2006;73(2):236–44.
[69]Oussalah M, Caillet S, Saucier L, Lacroix M. Inhibitory effects
of selected plant essential oils on the growth of four patho-
genic bacteria: E. coli O157:H7, Salmonella Typhimurium,
Staphylococcus aureus and Listeria monocytogenes. Food
Control. 2007;18(5):414–20.
[70]Lapčík L, Vašina M, Lapčíková B, Hui D, Otyepková E,
Greenwood RW, et al. Materials characterization of advanced
fillers for composites engineering applications. Nanotechnol
Rev. 2019;8(1):503–12.
[71]Sahari J, Sapuan SM, Zainudin ES, Maleque MA. Thermo-me-
chanical behaviors of thermoplastic starch derived from sugar
palm tree (Arenga pinnata). Carbohydr Polym. 2013
Feb;92(2):1711–6.
[72]Sanyang ML, Sapuan SM, Jawaid M, Ishak MR, Sahari J. Effect
of sugar palm-derived cellulose reinforcement on the me-
chanical and water barrier properties of sugar palm starch
biocomposite films. BioResources. 2016;11(2):4134–45.
[73]Acosta S, Jiménez A, Cháfer M, González-Martínez C, Chiralt A.
Physical properties and stability of starch-gelatin based films
as affected by the addition of esters of fatty acids. Food
Hydrocoll. 2015;49:135–43.
[74]Choi WS, Singh S, Lee YS. Characterization of edible film
containing essential oils in hydroxypropyl methylcellulose and
its effect on quality attributes of ‘Formosa’plum (Prunus sal-
icina L.). LWT. 2016 Jul;70:213–22.
[75]Peng Y, Li Y. Combined effects of two kinds of essential oils on
physical, mechanical and structural properties of chitosan
films. Food Hydrocoll. 2014 May;36:287–93.
[76]Sánchez-González L, Pastor C, Vargas M, Chiralt A, Gonzalez-
Martinez C, Chafer M. Effect of hydroxypropylmethylcellulose
and chitosan coatings with and without bergamot essential oil
on quality and safety of cold-stored grapes. Postharvest Biol
Technol. 2011;60(1):57–63.
[77]Ilyas RA, Sapuan SM, Ishak MR, Zainudin ES, Products F. Sugar
palm nanofibrillated cellulose fibre reinforced sugar palm
starch nanocomposite. Part 1: Morphological. Mechanical and
physical properties. 2018 September:1–30.
[78]Salzer UJ, Furia TE. The analysis of essential oils and extracts
(oleoresins)from seasonings –A critical review. C R C Crit Rev
Food Sci Nutr. 1977;9(4):345–73.
[79]Shankaranarayana ML, Raghavan B, Abraham KO,
Natarajan CP. Titrimetric determination of total aldehydes in
cinnamon bark and leaf oils using chloramine‐T reagent. J Food
Qual. 1981;4(1):35–41.
[80]Liu X, Xu Y, Zhan X, Xie W, Yang X, Cui SW, et al. Development
and properties of new kojic acid and chitosan composite bio-
degradable films for active packaging materials. Int J Biol
Macromol [Internet]. 2020;144:483–90. Available from:
https://doi.org/10.1016/j.ijbiomac.2019.12.126.
[81]Ahmad M, Hani NM, Nirmal NP, Fazial FF, Mohtar NF, Romli SR.
Optical and thermo-mechanical properties of composite films
based on fish gelatin/rice flour fabricated by casting tech-
nique. Prog Org Coatings [Internet]. 2015;84:115–27. Available
from: http://dx.doi.org/10.1016/j.porgcoat.2015.02.016.
[82]Xu YX, Kim KM, Hanna MA, Nag D. Chitosan-starch composite
film: Preparation and characterization. Ind Crops Prod.
2005;21(2):185–92.
1158 Razali M. O. Syafiqet al.
[83]Ilyas RA, Sapuan SM, Ishak MR, Zainudin ES. Development
and characterization of sugar palm nanocrystalline cellu-
lose reinforced sugar palm starch bionanocomposites.
Carbohydr Polym [Internet].
2018;202(September):186–202. Available from: https://
doi.org/10.1016/j.carbpol.2018.09.002.
[84]Noshirvani N, Ghanbarzadeh B, Gardrat C, Rezaei MR,
Hashemi M, Le Coz C, et al. Cinnamon and ginger essential oils
to improve antifungal, physical and mechanical properties of
chitosan-carboxymethyl cellulose films. Food Hydrocoll. 2017
Sep;70:36–45.
[85]Ma W, Tang C-H, Yin S-W, Yang X-Q, Wang Q, Liu F, et al.
Characterization of gelatin-based edible films incorporated
with olive oil. Food Res Int. 2012 Nov;49(1):572–9.
[86]Sun L, Sun J, Chen L, Niu P, Yang X, Guo Y. Preparation and
characterization of chitosan film incorporated with thinned
young apple polyphenols as an active packaging material.
Carbohydr Polym. 2017 May;163:81–91.
[87]Hosseini SF, Rezaei M, Zandi M, Farahmandghavi F. Bio-based
composite edible films containing origanum vulgare L.
essential oil. Ind Crops Prod. 2015 May;67:403–13.
[88]Tongnuanchan P, Benjakul S, Prodpran T, Pisuchpen S,
Osako K. Mechanical, thermal and heat sealing properties of
fish skin gelatin film containing palm oil and basil essential oil
with different surfactants. Food Hydrocoll. 2016
May;56:93–107.
[89]Turek C, Stintzing FC. Stability of essential oils: A review.
Compr Rev Food Sci Food Saf. 2013;12(1):40–53.
[90]Wong Y, Ahmad-Mudzaqqir M, Wan-Nurdiyana W. Extraction of
essential oil from cinnamon (cinnamomum zeylanicum). Orient
J Chem. 2014 Mar;30(1):37–47.
[91]Murbach Teles Andrade BF, Nunes Barbosa L, da Silva Probst I,
Fernandes Júnior A. Antimicrobial activity of essential oils.
J Essent Oil Res. 2014 Jan;26(1):34–40.
[92]Cardoso-Ugarte GA, López-Malo A, Sosa-Morales ME.
Cinnamon (Cinnamomum zeylanicum)essential oils. Essent
Oils Food Preserv Flavor Saf. 2016;339–47.
[93]Khalid H, Lêda RAF, EEO. Cinnamon oil. Green Pestic Handb
Essent Oils Pest Control [Internet]. 2017 Feb 7. 117–50. Available
from: https://www.qeios.com/read/definition/70017.
[94]El Atki Y, Aouam I, El Kamari F, Taroq A, Nayme K, Timinouni M,
et al. Antibacterial activity of cinnamon essential oils and their
synergistic potential with antibiotics. J Adv Pharm Technol Res.
2019;10(2):63–7.
[95]Kamaliroosta L. Extraction of cinnamon essential oil and
identification of its chemical compounds. J Med Plants Res
[Internet]. 2012 Jan 30;6(4):609–14. Available from: http://
www.academicjournals.org/jmpr/abstracts/abstracts/ab-
stracts2012/30Jan/Kamaliroosta et al.htm.
[96]Dierking Jim. Material safety data sheet cinnamomum essen-
tial oil [Internet]. Liberty natural products. 2020 [cited 2020
Oct 8].p.1–2. Available from: https://www.libertynatur-
al.com/msd/19.htm.
[97]Young C. Is cinnamon flammable? [Internet]. chefsteps. 2019
[cited 2020 Oct 8]. p. 1. Available from: https://www.chef-
steps.com/activities/is-cinnamon-flammable
Effect of CEO on starch biopolymer composites 1159
Content uploaded by S. M. Sapuan
Author content
All content in this area was uploaded by S. M. Sapuan on Dec 09, 2020
Content may be subject to copyright.
