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Article
Jean-François Fiset, Jean-François Blais et Patricio A. Riveros
Revue des sciences de l'eau/ Journal of Water Science
, vol. 21, n° 3, 2008, p. 283-308.
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"Review on the Removal of Metal Ions from Effluents Using Seaweeds, Alginate Derivatives
and Other Sorbents"
REVIEW ON THE REMOVAL OF METAL IONS FROM EFFLUENTS
USING SEAWEEDS, ALGINATE DERIVATIVES AND
OTHER SORBENTS
Revue sur l’enlèvenement des ions métalliques des efuents par l’utilisation des macro-algues, des dérivés d’alginate
et autres sorbants
Jean-François Fiset
1
*, Jean-François Blais
2
, Patricio a. riveros
1
1
Natural Resources Canada, CANMET-MMSL, 555 Booth Street, Ottawa, (Ont) K1A 0G1
2
*Auteur pour correspondance :
613-995-4641
: 613-996-9041
Courriel : jeset@nrcan.gc.ca
Revue des Sciences de l’Eau 21(3) (2008) 283-308
ABSTRACT
Biosorbents, especially those derived from seaweed
(macroscopic algae) and alginate derivatives, exhibit high
affinity for many metal ions. Because biosorbents are widely
abundant (usually biodegradable) and less expensive than
industrial synthetic adsorbents, they hold great potential for
the removal of toxic metals from industrial effluents. Various
studies have demonstrated the efficiency of living and non-
living micro-organisms, such as bacteria, yeasts, moulds,
micro-algae, cyanobacteria and biomass from water treatment
sewage to remove metals from solution. Several types of
organic and inorganic biomass have also been used as sorbent
materials. In addition, by-products from the forestry industry,
as well as agriculture waste and natural sorbents, have also been
studied. is paper reviews and summarizes some key recent
developments in these areas and it describes and discusses
some specific applications of selected natural sorbents.
Key Words: Metal, removal, adsorption, alginate, seaweed,
natural sorbent, wastewater, effluent, treatment.
RÉSUMÉ
Les biosorbants, particulièrement ceux préparés à partir des
algues macroscopiques et des dérivés d’alginate, démontrent une
très bonne capacité d’adsorption des ions métalliques toxiques.
Ces biosorbants étant facilement disponibles (biodégradable)
et moins coûteux que les adsorbants (industriels) synthétiques,
Metals adsorption on seaweed, alginate and other sorbents
ils présentent un grand potentiel d’utilisation pour l’enlèvement
des métaux toxiques des effluents industriels. Les récents
développements dans ce domaine ont été revus et font l’objet
de la présente synthèse. Des applications spécifiques sont
décrites et discutées.
Diverses technologies sont disponibles pour enlever les
métaux des effluents industriels tels que la précipitation
(sous forme d’hydroxydes ou de sulfures), la coprécipitation,
l’adsorption, l’extraction par solvant, la cémentation,
l’électrodéposition, l’électrocoagulation, l’échange d’ions et
les technologies de séparation membranaire. Néanmoins, la
plupart de ces techniques présentent des coûts d’exploitation
élevés et, dans certains cas, sont limitées en terme de rendement
d’élimination des métaux. Dans ce contexte, l’utilisation
d’adsorbants naturels (dérivés de matière organique ou
inorganique) constitue une alternative intéressante aux produits
synthétiques. De nombreux articles ont d’ailleurs été publiés au
cours des dernières années faisant état de la performance d’une
grande variété d’adsorbants naturels pour enlever les métaux
des effluents.
Plusieurs espèces d’algues marines ont aussi démontré des
propriétés pour adsorber les métaux, mais les algues marines
brunes, telles que Sargassum et Ascophyllum semblent avoir la
plus grande capacité de rétention des métaux, à cause de leur
grande concentration en polysaccharides. L’intégrité physique
des algues est également importante, ceci afin de prévenir
leur désintégration pendant les processus d’adsorption. Afin
d’améliorer la stabilité et les propriétés mécaniques des algues
fraîches, diverses méthodes ont été suggérées : i) greffage
dans des polymères synthétiques; ii) incorporation dans des
matériaux inorganiques; iii) liaison sur un support adéquat; et
iv) séquestration par un agent de liaison.
L’acide alginique est un polymère naturel se trouvant
dans les algues brunes. Ce polymère est extrait en traitant les
algues avec une solution de carbonate de sodium, puis l’acide
alginique est précipité, ou converti en sel d’alginate de calcium.
Lorsque l’acide alginique réagit avec des ions polyvalents,
tel que le calcium, une séquestration se produit procurant
un gel d’alginate ayant des forces structurales significatives.
L’alginate de calcium peut être préparé sous plusieurs formes,
telles que des billes, de la poudre, des membranes, des
fibres ou des supports d’immobilisation cellulaire. Les billes
sont particulièrement intéressantes du point de vue de leur
application et de leur réutilisation.
L’utilisation des algues marines en tant que procédé
d’enlèvement des métaux doit tenir compte de plusieurs
considérations techniques. Les systèmes de biosorption
utilisent les biomasses sous forme solide en un procédé
conventionnel de contact solide-liquide et, dans certains cas,
les systèmes comprennent plusieurs étapes de biosorption et de
désorption. L’effluent à traiter peut entrer en contact avec la
biomasse selon un procédé en mode discontinu, semi-continu
ou continu. Une fois saturés en métaux lourds, les adsorbants
peuvent être disposés de façon sécuritaire, ou être réutilisés
après élution des métaux. Dans ce cas, la plupart des métaux
lourds (Cd, Co, Cu, Mn, Pb, Zn) peuvent être élués à l’aide
d’acides dilués (chlorhydrique, sulfurique, nitrique) ou de
solutions salines concentrées. Certains métaux qui sont moins
dépendants du pH d’adsorption (Au, Ag, Hg) ne peuvent être
élués en utilisant un acide dilué. Des solutions de thiourée ou de
mercaptol peuvent être utilisées pour l’or et l’acétate de sodium
pour la récupération de l’argent. La combustion des algues est
également possible, néanmoins, elle n’est envisageable que si
l’adsorbant est peu dispendieux et grandement disponible.
Plusieurs types de biomasses organiques ou inorganiques
peuvent être utilisés comme matériaux adsorbants. Des études
ont démontré l’efficacité des microorganismes vivants ou morts
incluant les bactéries, les levures, les moisissures, les microalgues,
les cyanobactéries et les biomasses issues du traitement des eaux
usées (boues d’épuration). Les rejets de l’industrie forestière,
incluant les sciures et les écorces de bois riches en lignine et en
tannins, ont été également étudiés de façon intensive. Certaines
plantes aquatiques (Ceratophyllum demersum, Lemna minor,
Myriophyllum spicatum) ont également été évaluées pour leur
capacité en phytofiltration et phytoassainissement. D’autres
études ont été effectuées sur la performance de fixation des
métaux de la chitine, cette dernière étant un biopolymère
naturel très abondant, lequel est classé second après la cellulose
en terme d’abondance. Ce biopolymère se retrouve largement
dans l’exosquelette des crustacés et des coquillages. Le chitosan
est produit en effectuant la dé-acétylation de la chitine en milieu
alcalin. La mousse de tourbe, les déchets d’agriculture (résidus
de thé et de café, pelures de certains légumes, écailles de noix,
d’arachides, de cacao) et divers autres adsorbants de nature
inorganique (sable, argile, oxyde, zéolites) ont également été
étudiés pour la récupération des métaux en solution.
D’un point de vue économique, plusieurs méthodes existent
pour traiter les eaux usées. La sélection d’une méthode dépend
de plusieurs critères, tels que la compatibilité avec les opérations
existantes, les coûts d’exploitation, la flexibilité des procédés
afin de pouvoir traiter des variations de charges hydrauliques et
de concentrations de contaminants. La méthode doit être aussi
fiable, robuste et simple d’utilisation. Dans certains cas, des
économies substantielles peuvent être réalisées en faisant appel
à l’adsorption des métaux sur des biomasses, comparativement
aux procédés conventionnels, tel que la précipitation des
métaux.
Mots clés : métal, enlèvement, adsorption, alginate, algue,
eau usée, sorbant naturel, effluent, traitement.
J.-F. Fiset et al./ Revue des Sciences de l’Eau
INTRODUCTION
e preservation of the environment has become
increasingly important in view of the ecological problems
brought about by industrialization and urbanization. Lakes
and rivers are particularly vulnerable to contamination as
a result of the discharge of large quantities of effluents from
industries and municipalities. e presence of heavy metals,
such as cadmium, chromium, cobalt, copper, lead, mercury,
nickel, silver, tin and zinc in rivers and watercourses may cause
serious health problems to living organisms (ALLOWAY and
AYERS, 1993; WASE and FORSTER, 1997).
Consequently, the norms and regulations imposed on
industrial effluents are becoming increasingly stringent.
ese restrictions stem largely from recent advances in
the understanding of the behaviour of heavy metals in the
environment. Being non-biodegradable, toxic metals tend
to accumulate in lower plants and animals, thereby entering
the food chain (CHANG et al., 2003; LIPPMANN, 2000;
WATTS, 1998).
Various technologies are available to remove metal ions
from industrial effluents, including precipitation (usually
as metal hydroxide or sulphide) and coprecipitation,
sorption, solvent extraction, cementation, electrodeposition,
electrocoagulation, ion exchange, and membrane technology
(BLAIS et al., 1999; BROOKS, 1991; CHMIELEWSKI
et al., 1997; PATTERSON, 1989). However, most of these
techniques require expensive, usually toxic, reagents, and this
fact significantly increases the capital and operating costs. In
this context, biosorbents (i.e., ion exchangers and adsorbents
derived from organic matter) present an attractive alternative
to synthetic and chemical products because they are widely
available, generally biodegradable and relatively inexpensive.
e main characteristics and past applications of biosorbents
have been summarized and discussed by several researchers
(ATKINSON et al., 1998; BABEL and KURNIAWAN,
2003; BAILEY et al., 1999; FISET et al., 2000; KUYUCAK
and VOLESKY, 1988; VEGLIO and BEOLCHINI, 1997;
VOLESKY, 1990; VOLESKY and HOLAN, 1995; WASE and
FORSTER, 1997). is present review summarizes the recent
research carried out on the use of biosorbents, especially those
derived from seaweeds, as substrates to remove heavy metal
from solutions and effluents. e various systems, mechanisms
and results presented in the scientific literature are analyzed
and compared.
1. SEAWEED SORBENTS
1.1 Seaweed-derived sorbents
e ability of biosorbents derived from marine algae
to adsorb metal ions has been demonstrated by several
researchers (LEE and VOLESKY, 1997; LEUSCH et al., 1995;
VEGLIO and BEOLCHINI, 1997; VOLESKY and HOLAN,
1995; VOLESKY and PRASETYO, 1994; WILSON and
EDYVEAN, 1994).
According to FAO (2002), the world aquaculture production
of brown, red and green seaweeds in 2002 was approximately 5,
2.5 and 0.018 Megatons (wet basis), respectively. Whereas all
these seaweed species exhibit good metal adsorption properties,
the brown marine algae (Sargassum and Ascophyllum) have the
highest capacity for heavy metal ions because of their high
polysaccharide content (VOLESKY and HOLAN, 1995).
Tables 1 and 2 summarize the research carried out on the
adsorption of metal ions using various seaweed species.
KLIMMEK et al. (2001) compared the efficiency of
thirty strains of algae for their abilities to extract cadmium,
lead, nickel and zinc from aqueous solution. ese researchers
found that the cyanophyceae Lyngbya taylorii exhibited high
uptake capacities for the four metals. Similarly, VOLESKY and
HOLAN (1995) provide some 23 examples of algal biomass
metal adsorption.
e physical integrity of algae is important to prevent them
from disintegrating during the sorption process. HOLAN et al.
(1993) summarized various techniques used to improve the
stability and the mechanical properties of fresh biopolymers:
Grafting into synthetic polymers;
Entrapment into inorganic material;
Binding to a suitable carrier; and
Cross-linking.
1.2 Algins and alginates derivatives
Algins are salts of alginic acid, a natural polymer found
in brown algae (Phaeophyceae). is polymer is extracted by
treating the seaweed with a sodium carbonate solution and
recovered by precipitation as alginic acid and afterward as the
sodium salt. e alginic acid molecules have a complicated
structure. Figure 1 shows two of the main segments found in
alginic acid. e abundance of carboxylic, hydroxyl and oxo
•
•
•
•
Metals adsorption on seaweed, alginate and other sorbents
References Seaweeds Metals Studied parameters
ARAVINDHAN
et al. Turbinaria sp. Cr(III)
Pre-treated with H
2
SO
, CaCl
2
and
MgCl
2
AXTELL et al. (2003) Microspora sp.
study
BORBA
et al. Sargassum lipendula Ni(II)
mathematical modeling
CEPRIÁ
et al. Ulva rigida Au(III), Hg(II), Ag(I),
CHAISUKSANT
(2003)
Gracilaria sheri (red marine
algae)
Cd(II), Cu(II)
treated with CaCl
2
.
COSSICH
et al. Sargassum sp. Cr(III)
DA COSTA
and DE FRANÇA
Codium sp., Colpomenia sp.,
Gelidium sp., Padina sp.,
Sargassum sp., Ulva sp.
Cd(II)
Langmuir and Freundlich models, ion-
DA COSTA
et al. Sargassum sp.
Al(III), Ca(II), Cd(II),
Mg(II), Na(I), Zn(II)
GONG
et al. (2005) Spirulina maxima
concentration, Freundlich model,
desorption, pre-treated with CaCl
2
.
GUPTA
et al. (2001) Spirogyra sp. Cr(VI)
pH, Langmuir model
HOLAN et al.
Ascophyllum nosodum,
Fucus vesiculosus
Cd(II)
HOLAN and VOLESKY
Ascophyllum nosodum,
Fucus vesiculosus
KAEWSARN and YU (2001)
Padina sp. Cd(II)
KAEWSARN
et al. (2001) Durvillaea potatorum Cu(II)
EDTA)
KAEWSARN
(2002) Padina sp. Cu(II)
KHANI
et al Cystoseira indica U(VI)
algae
KRATOCHVILL
et al. Sargassum sp. Cr(III), Cr(VI) Protonated seaweed, pH optimization
KUYUCAK
and VOLESKY
Ascophyllum nodosum,
Chondrus crispus, Halimeda
opuntia, Palmaria palmata,
Porphyra tenera, Sargassum
natans
Ag(I), Au(III), Cd(II),
U(VI), Zn(II)
KUMAR
et al. Ulva fasciata sp. Cu(II)
LAU
et al. (2003) Ulva lactuca Cu(II), Ni(II), Zn(II)
Table 1. Studies on the metal sorption using seaweeds
Tableau 1. Études portant sur l’adsorption des métaux par utilisation d’algues macroscopiques
J.-F. Fiset et al./ Revue des Sciences de l’Eau
References Seaweeds Metals Studied parameters
LEE
and VOLESKY Sargassum uitans
Al(III), Ca(II), K(I),
Mg(II), Na(I)
LEUSCH
et al.
Ascophyllum nodosum
Sargassum uitans
Cd(II), Cu(II), Ni(II),
polyethylene imine, Langmuir,
LODEIRO
et al. Cystoseira baccata
LUO
et al. Laminaria japonica
MATHEICKAL
et al. Ecklonia radiata Cu(II)
MATHEICKAL
Phellinus badius
NAJA
and Sargassum uitans Cu(II), Zn(II), Cd(II)
OFER
et al. (2003)
Padina pavonia,
Sargassum vulgaris Cd(II), Ni(II)
Kinetic studies, desorption studies,
Langmuir isotherm
PARK
et al. Ecklonia sp. Cr(III), Cr(VI)
FTIR characterization
PRASHER
et al. Palmaria palmate (red algae)
Cd(II), Cu(II), Ni(II),
Freundlich, Langmuir and Brunauer
Emmer and Teller (BET) models,
concentration and temperature
SENTHILKUMAR
et al.
Gracilaria crassa, Gracilaria
edulis, Hypnea valentiae, Ulva
lactuca, Ulva reticula, Codium
tomentosum, Chaetomorpha
antennina, Turbinaria conoides,
turbinaria ornata, Sargassum
polycystium
Zn(II)
Freundlich, Redlich-Peterson and
desorption studies
TSUI
et al. Sargassum hemiphyllum
Ag(I), As(V), Cd(II),
Co(II), Cd(II), Cr(III),
Cr(VI), Mn(II), Ni(II),
VOLESKY
Sargassum natans, Sargassum
uitans, Sargassum vulgaris,
Ascophyllum nodosum,
Palmaria palmata, Chondrus
crispus, Halimeda opuntia,
Fucus vesiculosis, Padina
gymnospora, Codium taylori
YU
et al.
Ascophyllum nodosum,
Lessonia avicans, Lessonia
nigresense
Laminaria japonica, Laminaria
hyperbola, Ecklonia maxima,
Ecklonia radiate, Durvillaea
potatorum
U(VI)
Metals adsorption on seaweed, alginate and other sorbents
groups gives alginic acid and alginate salts strong chelating
properties for metal ions.
When alginic acid reacts with polyvalent ions, such as
calcium, a cross-linking effect takes place, which gives the
resulting alginate gel a significant structural strength (NESTLE
and KIMMICH, 1996). e cross-linking is caused by a
polyvalent ion binding two or more carboxylic groups on
adjacent polymer chains, and this can be accompanied by
chelation of the ion by the hydroxyl and carboxyl groups of the
polymer chains (SHIMIZU and TAKADA, 1997).
e alginate products are not only used for metal removal,
but also for other commercial applications, including some in
the food industry (HOLAN et al., 1993; RENN, 1997). e
main advantage of using algae or biomass derivatives is that they
do not require nutrients and they are resistant to the physical-
chemical properties of heavy metal solutions (ARAÚJO and
TEIXEIRA, 1997). Alginate products have been used as
supporting substrate for a variety of active agents, including
microorganisms, algae (AL-RUB et al., 2004; SINGHAL et al.,
2004), chitosan (GOTOH et al., 2004; HUANG et al., 1996),
activated sludge (WANG et al., 2004), cellulose and humic
acid (MISRA and PANDEY, 2001). Tables 3 and 4 present
alginate derivatives studied for their capacity to adsorb different
metals.
Calcium alginate may be prepared in various forms, such
as beads, powder (CRIST et al., 1994), membranes (HIRAI
and ODANI, 1994; TOTI and AMINABHAVI, 2002) or
fibers (SHIMIZU and TAKADA, 1997; WILLIAMS and
EDYVEAN, 1997) and can be used as cell-immobilization
support (IBÁÑEZ and UMETSU, 2002). Bead particles have
practical advantages in terms of applicability to a wide variety
of process configuration and reusability (GOTOH et al., 2004).
Also, the alginate beads may be protonated (IBÁÑEZ and
UMETSU, 2002, 2004) or doped with another metallic ion
to obtain various bead properties (MIN and HERING, 1998).
GOTOH et al. (2004) improved the mechanical strength and
resistance to chemical and microbial degradation without
affecting adsorption capacity by cross-linking the alginate
beads with 1,6-Diaminohexane. Producing alginate gels “in-
situ” is also feasible when a high concentration of metal ions is
References Sorbents Cd(II) Cu(II) Cr(III) Ni(II) Zn(II)
ARAVINDHAN
et al. T. ornata 31
CHAISUKANT (2003) G. sheri
COSSICH
et al. Sargassum sp.
KUMAR
et al. Ulva fasciata sp.
LAU
et al.(2003)
Ulvas sp. 1
Ulva lactuca
Ulva sp. 3
55
51
10
31
LODEIRO
et al. S. muticum
LODEIRO
et al C. baccata 101
OFER et al. (2003)
S. vulgaris
P. pavonia
135
PAVASANT
et al. Caulerpa lentillifera
Table 2. Recent studies on the adsorption capacities (mg/g) of marine algae for selected heavy metals.
Tableau 2. Études récentes sur la capacité d’adsorption (mg/g) des l’algues marines pour des métaux lourds sélectionnés.
O
HO
COO
-
HO
O
O
HO
COO
-
O
HO
O
HO
COO
-
HO
O
O
HO
COO
-
O
HO
O
HO
COO
-
HO
O
O
HO
COO
-
O
HO
O
HO
COO
-
HO
O
O
HO
COO
-
O
HO
O
HO
COO
-
HO
O
O
HO
COO
-
O
HO
O
O
OH
HO
COO
-
O
HO
O
OH
COO
-
O
O
OH
HO
COO
-
O
HO
O
OH
COO
-
O
O
O
OH
HO
COO
-
O
HO
O
OH
COO
-
O
O
OH
HO
COO
-
O
HO
O
OH
COO
-
O
A
B
Figure 1. Main segments of alginic acid: A) a poly(D-mannuronosyl
segment and B) a poly(L-guluronosyl) segment.
Principales parties de l’acide alginique : A) une
portion poly(D-mannuronosyl, et B) une portion
poly(L-guluronosyl).
J.-F. Fiset et al./ Revue des Sciences de l’Eau
References Sorbents Metals Studied parameters
AL-RUB
et al. Ni(II)
model, sorption desorption cycle
AKSU
et al.
Chlorella vulgaris
Cu(II)
CHEN
et al. Cu(II)
CRIST
et al
Vaucheria, Rhizoclonium,
Ca-alginate powder
Ag(II), Al(III),
Ba(II), Cd(II),
Cu(II), La(III),
Zn(II)
FOUREST
and VOLESKY
Sargassum uitans, Ascophyllum
nodosum, Fucus vesiculosus,
Laminaria japonica
Ca(II), Cd(II),
Cu(II),
and
13
GOTOH
et al Cu(II), Mn(II)
and SEM characterization
HIRAI
and ODANI
Co(II)
HUANG
et al. Cu(II), Ni(II)
IBÁÑEZ
and UMETSU
(2002)
Co(II), Cr(III),
Cu(II),
Ni(II), Zn(II)
strength, pH and protonation
IBÁÑEZ
and UMETSU
Protonated dry alginate
Cr(III)
EPMA-EDX analysis
JANG et al. Co(II), Cu(II)
JANG et al. Cu(II), Zn(II)
JEON et al. (2002)
,
FTIR and
13
C NMR characterization,
elemental analysis, desorption
JEON et al. (2005)
KARAGUNDUZ
et al. Cu(II)
LU and WILKINS
Sacharomyces cerevisiae
Cd(II), Cu(II),
Zn(II)
Caustic treatment, metal desorption,
NESTLE
and KIMMICH
Cu(II)
PAPAGEORGIOU
et al.
Laminaria
digitata
PARK
and CHAE
capsules, alginate gel coated
SEM characterization
Table 3. Studies on the metal sorption using alginate products.
Tableau 3. Études portant sur l’adsorption des métaux sur les produits d’alginate.
Metals adsorption on seaweed, alginate and other sorbents
SEKI and SUZUKI Alginic acid and humic acid
model
SHIMIZU
and TAKADA
Bi(III), Cu(II),
characterization
SINGHAL
et al. Chlorella pyrendoidosa
alginate
U(IV), U(VI)
characterization
VEGLIO
et al. (2002) Cu(II)
present in solution (ARAÚJO and TEIXEIRA, 1997; JANG
et al., 1999).
Various chemical treatments may be applied on alginic
acid in order to increase metal uptake capacity such as
carboxylation, phosphorylation, and sulfonation (JEON et al.,
2002), although these treatments tend to increase the cost of
the resulting product.
ARAÚJO and TEIXEIRA (1997) studied the transport
properties of Cr(III) on alginate beads using the Linear
Adsorption model and the Shrinking Core model. For low
Cr(III) concentration, ion exchange was the rate-controlling
mechanism and the experimental results fit well with the
Shrinking Core model. At higher concentrations, however, the
Linear Adsorption model was a better fit for the experimental
results and ionic exchange was no longer the main mechanism
of sorption. e study of CHEN et al. (1993) indicated that
Linear Adsorption model was preferable for the Cu calcium
alginate gel.
1.3 Algal biosorption systems
Engineering considerations are very important during the
development of an algal-based sorption system. All biosorption
systems used biomass in solid form in a basic solid-liquid contact
process, with, in certain cases, cycling of the process through
biosorption and desorption stages (GARNHAM, 1997). e
effluent to treat would make contact with the biosorbent in
a batch, semi-continuous or continuous flow system. e
following reactor types have been described by BANKS (1997)
as potential biosorption systems:
• Conventional stirred tank reactors;
• Packed bed reactors (upflow and downflow);
• Expanded bed reactors;
• Fluidised bed reactors;
• Airlift reactors.
In the cases of algal-based processes using actively growing
biomass these can also be based on ponds, lagoons, streams and
artificial stream meander units (VOLESKY, 1990).
References Sorbents Cu(II) Cr(III) Cr(VI) Ni(II) Pb(II)
AL-RUB
et al.
Free dead algal cell
31
BAJPAI
et al
Bio-polymeric (Ca and
gelatin)
112
NGOMSIK
et al.
Magnetic alginate
microcapsule
OZDEMIR
et al. (2005)
polysaccharide
Alginate capsule
Table 4. Recent studies on the adsorption capacities (mg/g) of alginate for selected heavy metals.
Tableau 4. Études récentes sur la capacité d’adsorption (mg/g) de l’alginate pour des métaux lourds sélectionnés
.
J.-F. Fiset et al./ Revue des Sciences de l’Eau
1.4 Adsorption mechanisms
e chemical structure and metal sorption mechanisms
of biomass have been extensively studied. VEGLIO and
BEOLCHINI (1997) classified the biosorption mechanisms
into two main categories, according to their cell functionality,
i.e., metabolism-dependant and non-metabolism-dependant.
e metabolism-dependant mechanism involves transport
across the cell membrane and a precipitation step (BRIERLEY,
1990; COSTA and LEITE, 1990), whereas the non-
metabolism-dependant mechanism consists of precipitation
(HOLAN et al., 1993; SCOTT and PALMER, 1990),
physical adsorption (AKSU et al., 1992; ZHOU and KIFF,
1991), ion exchange (FRISS and MYERS-KEITH, 1986;
MURALEEDHARAN and VENKOBACHAR, 1990) and
complexation (CABRAL, 1992; TSEZOS and VOLESKY,
1981). Another way to classify the mechanism is based
on the location where the extracted metal accumulates;
for example, there is intracellular accumulation (transport
across membrane), cell surface adsorption/precipitation (ion
exchange, complexation, physical adsorption, precipitation)
and extra-cellular accumulation/precipitation (VEGLIO and
BOELCHINI, 1997).
1.5 Adsorption models
Various models have been used to evaluate the experimental
data in order to identify the sorption mechanisms, i.e.,
chemisorption, physical adsorption or ion exchange. Some
studies have compared the ion exchange model with the
Langmuir adsorption model (DA COSTA and DE FRANÇA,
1996; FIGUEIRA et al., 2000). e Langmuir adsorption
model assumes that only one type of adsorption site exists
(i.e., all surface sites have equal activity) and that adsorption
equilibrium is reached with the formation of a monolayer
(STUMM and MORGAN, 1996). is model does not take
into account the speciation of the metal in solution and,
therefore, it applies only if the ionic strength, the pH and the
ligand concentration are constants.
e ion exchange model has been found to give the best
fit for metal sorption on algae biomass because the sorption is
accompanied by the release of ions (e.g., Ca
2+
, Mg
2+
, Na
+
and K
+
)
(CRIST et al., 1994; KRATOCHVIL et al., 1998; KUYUCAK
and VOLESKY, 1988; SCHIEWER and VOLESKY, 1995).
Experiments have been carried out to study several system
variables, such as the initial concentration (CRIST et al., 1994),
the sorbent particle size (FISHER, 1985), and the solution pH
(JANG et al., 1995; LEE and VOLESKY, 1997). Similarly,
experimental data have been analyzed to determine the reaction
kinetic order of a pore/solid phase diffusion mechanism (HO
and MCKAY, 2000).
Other models used to describe various biosorption
isotherms include the Freundlich model, a combination of the
Langmuir and Freundlich models, the Radke and Prausnitz
model, the Reddlich-Peterson model, the Brunauer (BET)
model, and the Dubinin-Radushkevich model (VOLESKY,
2003). e «Ideal Absorbed Solution eory» (IAST) and the
«Surface Complexation» (SCM) models have also been used
for solutions containing a mixture of metal ions (VOLESKY,
2003). Some other structured types of models taking into
consideration the metal speciation in solution, the pH and
the electrostatic attraction in solution have been proposed by
SCHIEWER and WONG (1999) and YANG and VOLESKY
(2000).
1.6 Metal recovery
e metal-laden biosorbent can be either eluted and
reused or disposed of in a safe manner. In the former case, the
biosorbent operates much like an ion exchange resin. Metals
can be eluted using a specific solution (the eluant) to generate a
small volume of a concentrated solution (the eluate). e choice
of eluant depends on the metal ion to be eluted. Common and
heavy metals (e.g., Cd, Co, Cu, Mn, Pb, Zn) are usually eluted
with dilute mineral acids (e.g., HCl, H
2
SO
4
, and HNO
3
) or
concentrated saline solutions (e.g. 0.5 M NaCl) (GARNHAM
et al., 1992b). EDTA has been used in certain cases, but it is
generally more expensive than mineral acids or saline solutions
(HORIKOSHI et al., 1979). e adsorption of some noble
metals, such as gold, silver and mercury, shows little or no
dependence on pH and, consequently, these metals cannot be
removed with dilute acid solutions (EDYVEAN et al., 1997).
iourea or mercaptoethanol solutions have been used for
recovering gold from biosorbents (DARNALL et al., 1986;
GREENE and DARNALL, 1990). Similarly, sodium acetate
solutions are effective for eluting copper and silver (HARRIS
and RAMELO, 1990). Sodium carbonate has been used to
desorb uranium from the algae Chlorella regularis (NAKAJIMA
et al., 1982).
In general, biosorbents decompose and char at relatively
low temperatures. erefore, metal-laden biosorbents can be
readily burned to produce an ash residue having a high metal
concentration. is alternative may be economically viable
for systems dealing with valuable metals and/or inexpensive
biosorbents (GARNHAM, 1997). Alginic acid powder and
calcium alginate beads have high affinity and capacity sorption
for Fe(III), and the extraction of Fe(III) from acid synthetic
solution is technically feasible (RIVEROS et al., 2001). Applied
to acid mine drainage, the Fe(III) extraction would result
in a significant reduction of the lime consumption and the
volume of the neutralization sludge (RIVEROS, 2004). Once
adsorbed, the Fe may be eluted and precipitated as hematite in
Metals adsorption on seaweed, alginate and other sorbents
order to obtain marketable and useful product (DUTRIZAC
and RIVEROS, 1999).
1.7 Cost analyses
Preliminary costing evaluation for biosorption treatment
options were conducted by ADERHOLD et al. (1996) and
VOLESKY (1999). e results indicate that biosorption is
a cost-effective technology. e cost-benefit analysis of any
treatment option presents various difficulties, such as the lack of
publicly available information on operating cost and the long-
term impact of the treatment operation. is is particularly
true for biotechnological processes. However, a comparative
cost study was conducted for biosorptive processes with ion
exchange and chemical precipitation (ECCLES, 1995). e
selection of an effluent treatment system needs to comply with
various criteria, such as compatibility with existing operations,
cost effectiveness, flexibility to handle fluctuation in quality
and quantity of effluent feed. e system should also be
reliable, robust, selective and simple (ECCLES, 1995). Eccles
compared the AMT-Bioclaim-process-based hard granular
biomass, Bacillus subtilis (BRIERLEY et al., 1986) with the
chemical precipitation method. e predicted results showed
that the AMT-Bioclaim method could reduce the cost per
gallon by over 50% when compared with a chemical treatment
method. A second study was completed by the author to
compare the Biofix process with chemical precipitation to treat
acid mine drainage. e Biofix process consists of a mixture
of biomass including bacteria, algae and fungi immobilized in
polyethylene beads. Using the data from JEFFERS (1994), the
acid mine drainage (AMD) treatment cost was 1.4 US$ per
1000 US gallons for the Biofix process and for conventional
lime treatment, it was calculated the cost would correspond to
1.5 US$ (ECCLES, 1995). Table 5 summarizes the treatment
options, along with their advantages and disadvantages.
2. OTHER NATURAL SORBENTS
Several research papers have been published about the use of
a variety of natural sorbents to remove metals from synthetic or
industrial effluents. Table 6 shows different studies conducted
on the utilization of natural sorbents for the removal of several
metals (Ag, Al, As, Au, Ba, Bi, Ca, Cd, Co, Cr, Cu, Fe, Hg, Ir,
Mg, Mn, Mo, Na, Ni, Os, Pb, Pd, Pt, Ra, Sb, St, Ti, Tl, V, Zn,
Zr), lanthanides (Ce, Eu, La, Yb) and actinides (, U).
2.1 Microorganisms
Many studies have been carried out on the utilization of
dead or living microorganisms, including bacteria, yeasts,
fungi, microalgae, cyanobacteria and activated sludge biomass
for metal removal from solutions. Some examples of different
microorganisms used for their metal adsorption capacity are
Treatment options Advantages Disadvantages
Lime precipitation
No sludge production
Electrolysis allows metal recycling
High capital and operating costs
solution
Osmosis
Very specialized application
conditions
Adsorption processes Versatile, simple
Low cost technology
Table 5. Treatment options for the removal of heavy metals (adapted from ADERHOLD et al., 1996).
Tableau 5. Options de traitement pour l’enlèvement des métaux (adapté d’ADERHOLD et al., 1996).
J.-F. Fiset et al./ Revue des Sciences de l’Eau
Metals References
Aluminium (Al) (III) CRIST
et al.ORHAN and BÜYÜKGÜNGÖRet al.
COUPAL and LALANCETTEMASRI and FRIEDMAN
Arsenic (As) (II, V) LOUKIDOU
et al. (2003), MASRI and FRIEDMAN
Barium (Ba) (II) CRIST
et al.SMITH et al.
Bismuth (Bi) (III) MASRI
and FRIEDMANSHIMIZU and TAKADA
Cadmium (Cd) (II) VOLESKY
and PRASETYOet al.
Calcium (Ca) (II) FISET
et al. (2002), FOUREST and VOLESKY
Cerium (Ce) (III) MASRI
and FRIEDMAN
Chromium (Cr)(III, VI) BAILEY
et al.FISHER et al.
FLYNN et al.KUYUCAK and VOLESKY
Copper (Cu) (I, II) MCKAY
et al.et al.et al.
Europium (Eu) (III) ANDRES
et al.
Gold (Au) (III) KUYUCAK
and VOLESKY NAKAJIMA (2003)
Iridium (Ir) (IV) RUIZ
et al. (2003)
Iron (Fe) (II, III) FISET
et al. (2002), NASSAR et al.et al.
Lanthanum (La) (III) BLOOM
and MCBRIDECRIST et al.
HOLAN and VOLESKYet al.MURATHAN and BÜTÜN
Magnesium (Mg) (II) CRIST
et al.FISET et al. (2002), CUI et al.
Manganese (Mn) (II) FISET
et al. (2002), NASSAR et al.et al.
Mercury (Hg) (I, II) FISHER
et al.VIRARAGHAVAN and KAPOOR
GUIBAL et al.SAKAGUSHI et al.
FLYNN et alLEUSCH et al.
Osmium (Os) (IV) RUIZ
et al. (2003)
Palladium (Pd) (II) BABA
and HIRAKAWA GUIBAL et al. (2001)
Platinum (Pt) (IV) BABA
and HIRAKAWAGUIBAL et al. (2001)
Radium (Ra) (II)
and
FISHER et al. FLYNN et al.
Sodium (Na) (I) FISET
et al. (2002), SPINTI et al.
Strontium (Sr) (II) SHIMIZU
and TAKADA SMALL et al.
Technetium (Tc) (VII) GARNHAM
et al.
Thallium (Tl) (I) MASRI
and FRIEDMAN
Thorium (Th) (IV) MASRI
and FRIEDMANTSEZOS and VOLESKY
Titanium (Ti) (IV) PARKASH
and BROWN
Uranium (U) (IV, VI) GUIBAL
et al.TSEZOS and VOLESKY
Vanadium (V) (V) GUIBAL
et al.
ANDRES et al.
Zinc (Zn) (II) ARTOLA
and RIGOLAKUYUCAK and VOLESKY
Zirconium (Zr) (IV) GARNHAM
et al.PARKASH and BROWN
Table 6. Studies on the adsorption of different metals using natural adsorbents.
Tableau 6. Études portant sur l’adsorption de différents métaux sur des adsorbants naturels.
Metals adsorption on seaweed, alginate and other sorbents
presented in Table 7. e metal adsorption on the cell surface of
non-living microorganisms usually involves different functional
groups such as carboxyl, amino, hydroxyl, sulfhydryl, phosphate
and sulfate groups (KAPOOR and VIRARAGHAVAN, 1997;
URRUTIA, 1997).
2.2 Forestry industry wastes
Forestry industry wastes including sawdust and tree
barks, which are lignin/tannin-rich materials, have been
also intensively studied for metal recovery from solutions
(FISET et al., 2000; SEKI et al., 1997; VAISHYA and PRASAD,
1991). e polyhydroxy polyphenol groups of tannin are
thought to be the active species in the metal adsorption (ion-
exchange) process (VASQUEZ et al., 1994). Lignin extracted
from black liquor, a waste product of the paper industry, has
been considered for metal adsorption, specifically Hg, Pb and
Zn (MASRI et al., 1974; SRIVASTAVA et al., 1994). Lignin
(Figure 2) contains polar functional groups, such as alcohols,
acids, aldehydes, ketones, phenol hydroxides and ethers, which
have varying metal binding capabilities (BAILEY et al., 1999).
Microorganisms References
Bacteria
Bacillus subtilis and spp. BEVERIDGE et al.COTORAS et al.
Micrococcus spp. COTORAS et al.LO et al. (2003)
Mycobacterium spp. ANDRES et al.
Pseudomonas spp. CABRALLOPEZ et al. (2002), D’SOUZA et al.
Streptomyces spp. FRISS and MYERS-KEITHMATTUSCHKA and STRAUBE
Zooglea ramigera AKSU et al.NORBERG and PERSSON
Yeasts
Candida spp. AKSU and DONMEZ (2001)
Candida utilis KUJAN et al.
Saccharomyces cerevisiae KUYUCAK and VOLESKYVOLESKY et al.
Fungi
Aspergillus niger VENKOBACHAR
Aureobasidium pullulans GADD and DE ROME
Cladosporium resinae GADD and DE ROME
Funalia trogii ARICA et al.
Ganoderma lucidum VENKOBACHAR
Penicillium spp. LOUKIDOU et al. (2003), SAY et al. (2003)
Rhizopus arrhizus FOUREST and ROUXTSEZOS and VOLESKY
Trametes versicolor BAYRAMOGLU et al. (2003)
Micro-algae
Chlorella vulgaris and spp. AKSU and ACIKELMEHTA et al. (2002)
Chlamydomonas spp. GARNHAM et al.SAKAGUCHI et al.
Eudorina spp. TIEN (2002)
Euglena spp. MANN et al.
Scenedesmus spp. GARNHAM et al.SAKAGUCHI et al.
Synechocystis aquatilis ERGENE et al
Cyanobacteria
Anabaena spp. GARNHAM et al.TIEN (2002)
Nostoc spp. FERNANDEZ-PINAS et al.HASSETT et al.
Oscillatoria spp. FISHER et al.TIEN (2002)
Synechoccus spp. GARNHAM et al.SAKAGUCHI et al.
Other
ARTOLA and RIGOLA HAMMAINI et al. (2003)
Table 7. Some examples of the microorganisms studied for the metal recovery from solutions.
Tableau 7. Exemples de microorganismes étudiés pour la récupération de métaux en solution.
J.-F. Fiset et al./ Revue des Sciences de l’Eau
2.3 Aquatic plants
Some aquatic plants (e.g. Ceratophyllum demersum, Lemna
minor, Myriophyllum spicatum) have also been tested for
phytoremediation or phytofiltration of metal-contaminated
effluents (AXTELL et al., 2003; KESKINKAN et al., 2004
SCHNEIDER et al., 2001). Chemical modification and
spectroscopic studies have shown that the cellular components
include carboxyl, hydroxyl, sulfate, sulfhydryl, phosphate,
amino, amide, imine, and imidazol moieties, which have metal
binding properties and are, therefore, the functional groups in
these plants (GARDEA-TORRESDEY et al., 2004).
2.4 Chitin and chitosan
Various researchers have utilized chitin and chitosan for
removing metal ions from effluents (MCKAY et al., 1989;
HSIEN and RORRER, 1995). Chitin (Figure 3) is the second
most abundant natural biopolymers after cellulose (BABEL
et al., 2003). is natural biopolymer is widely found in the
exoskeleton of shellfish and crustaceans (KIM and PARK, 2001).
Chitosan (Figure 4) is produced by alkaline N-deacetylation of
chitin. Crab shells or seafood processing waste sludge can also
be used directly for metal adsorption without chitin extraction
(KIM and PARK, 2001; LEE and DAVIS, 2001). e metal
ions adsorption on chitosan mostly involved free amine groups.
However, the binding ability of these sorbents for various metal
ions is not directly proportional to the degree of free amine
content (EDYVEAN et al., 1997).
2.5 Peat moss
Peat moss, which is also very abundant in nature, has been
intensively studied for water decontamination and particularly
for the metal removal from waste streams (KERTMAN et al.,
1993; SHARMA and FORSTER, 1993; VIRARAGHAVAN
and RAO, 1993). Peat moss is a complex material, having lignin
and cellulose as its major components. Both these components
contain polar functional groups, such as carboxylic acids,
phenol hydroxides, alcohols, aldehydes, ketones and ethers,
which bind metal ions (BROWN et al., 2000. COUILLARD,
1994; WASE et al., 1997).
2.6 Agricultural wastes
Other types of natural sorbents proposed in the literature
for metal retention include different agricultural wastes (e.g.,
tea/coffee and rice residues, fruit and vegetable peels, nut
skins/husks). Some examples of these inexpensive and readily
available materials are presented in Table 8. e polyhydroxy
polyphenol groups, as well as, carboxylic and amino groups,
found in these materials are involved in the metal adsorption
(ion-exchange) process (MEUNIER et al., 2003b; RANDALL
et al., 1974).
2.7 Miscellaneous sorbents
Finally, other natural sorbents studied include notably animal
bones (BANAT et al., 2002), clays (e.g. bentonite, kaolinite,
C
OCH
3
O
C
C
HC
HOCH
2
HCOH
OCH
3
O
HOCH
2
OCH
3
O
Figure 2. e chemical structure of lignin.
Structure chimique de la lignine.
O
O
NHCOCH
3
HO
OH
O
O
NHCOCH
3
HO
OH
Figure 3. e chemical structure of chitin.
Structure chimique de la chitine.
O
O
NH
2
HO
OH
O
O
NH
2
HO
OH
Figure 4. e chemical structure of chitosan.
Structure chimique du chitosan.
Metals adsorption on seaweed, alginate and other sorbents
montmorillonite, wollastonite) (CELIS et al., 2000; PRADAS
et al., 1994), human hair and teeth (HELAL et al., 2002;
TAN et al., 1985), leaf mould (SHARMA and FORSTNER,
1994), sand (AWAN et al., 2003), metal oxides (Al, Fe, Mn
– oxides) (BAILEY et al., 1992; TRIVEDI and AXE, 2001),
vermicompost (PEREIRA and ARRUDA, 2003), xanthate
(FLYNN et al., 1980; JAWED and TARE, 1991), and zeolites
(e.g., clinoptilolite and chabazite) (GENÇ-FUHRMAN, 2007;
LEPPERT, 1990; KALLO, 2001; OLIVEIRA et al., 2004).
2.8 Industrial applications
e majority of studies on metal adsorption on biosorbents
have been carried out using synthetic solutions containing one
or several metal ions (BLAIS et al., 2003; CRIST et al., 1994;
MASRI and FRIEDMAN, 1974). However, many research
papers have shown the efficiency of biosorbents for the removal
of metal ions from industrial wastewaters and acid mine drainage
solutions (MCGREGOR et al., 1998; UTGIKAR et al., 2000;
ZOUMIS et al., 2000), landfill leachates (ABOLLINO et al.,
2003; CECEN and GURSOY, 2001), tannery wastewaters
(ALVES et al., 1993), electroplating effluents (AJMAL et
al., 1996, 2000; ALVAREZ-AYUSO et al., 2003; LO et al.,
2003), acid leachates from sewage sludge decontamination
(FISET et al., 2002), acid leachates from soil decontamination
(MEUNIER et al., 2004), and alkaline leachates from
air pollution control residues from municipal solid waste
incinerators (BLAIS et al., 2002a, BLAIS et al., 2002b).
Biosorption has proved to be effective for removing
metal ions from contaminated solutions and effluents. e
main advantages of biosorption over conventional treatment
techniques include lower capital and operating costs, arising
from the use of abundant and inexpensive natural products,
and lower disposal cost of the spent adsorbents because of
their biodegradable nature. However, industrial applications
of biosorption are rare, and this situation has been attributed
to the non-technical gaps involved in the commercialization
of technological innovations (VOLESKY and NAJA, 2005).
Furthermore, most biosorption studies have been conducted
in batch systems, rather than in the continuous systems that
are typical of industrial applications, such as fluidized bed
and packed bed columns and continuous stirred tank reactors
(MEHTA and GAUR, 2005). Despite these facts, VOLESKY
Wastes References
Banana pith and peels ANNADURAI et al. (2003), LOW et al.
Canola meal AL-ASHEH and DUVNJAK
Carrot residues NASERNEJAD et al. (2005)
ABIA et al.
AL-ASHEH et al. (2002)
Cocoa shells FISET et al. (2002), MEUNIER et al.
RANDALL et al. OFOMAJA andet al
MINAMISAWA et al. (2002)
BOSINCO et al.GOLDBERG and GRIEVE (2003)
FIOL et al.ESCUDERO et al
Indian mustard CRIST
et al.
MARSHALL and CHAMPAGNE
Nut and walnut shells ORHAN and BÜYÜKGÜNGÖR
GHARAIBEH
et al.VEGLIO et al. (2003)
Onion peels KUMAR and DARA
Orange peels AJMAL et al. (2000), MASRI et al.
HO
CHAMARTHY et al. (2001), RANDALL et al.
and SAEED (2002)
AJMAL et al. (2003), MONTANHER et al. (2005)
Sheep manure wastes AL-RUB et al. (2003)
OZDEMIR et al.
ORHAN and BÜYÜKGÜNGÖRTEE and KHAN
Table 8. Agricultural wastes studied for the metal recovery from solutions.
Tableau 8. Déchets agricoles étudiés pour la récupération de métaux en solution.
J.-F. Fiset et al./ Revue des Sciences de l’Eau
and NAJA (2005) have identified some industrial operations
which represent a big potential market for biosorption
applications; these include electroplating and metal finishing,
mining and ore processing, smelting, leather processing and
printed circuit board manufacturing. However, as some
of these sectors may be reluctant to novel biotechnology
applications, biotechnology industries may have to share the
risk with the industry. erefore, biotechnology industry may
have to develop partnership with industries in order to finance,
build and operate the treatment plant or to provide a turnkey
operating plant.
CONCLUSIONS
Biosorbents, especially those derived from seaweed and
alginic acid, have attracted much interested in recent years
as a source of inexpensive adsorbents for toxic metallic ions.
Biosorbents are widely available in nature, can be readily
produced under various forms, and are both non-toxic and
biodegradable. ese characteristics give them a definitive
advantage over synthetic products for the removal of toxic
metals from industrial effluents. e physical stability of
biosorbents, especially in alkaline conditions continues to be a
drawback and more research is needed in this area.
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