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ISSN 1615-9306 · JSSCCJ 39 (6) 1017–1212 (2016) · Vol. 39 · No. 6 · March 2016 · D 10609

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Chromatography · Electroseparation

Applications
Biomedicine · Foods · Environment
1152 J. Sep. Sci. 2016, 39, 1152–1159

Mohd Marsin Sanagi1,2 Review Article

Saw Hong Loh3
Wan Nazihah Wan Ibrahim1,4
Neda Pourmand1
Ahmed Salisu1
Wan Aini Wan Ibrahim1
Imran Ali5*
1 Department of Chemistry,
Faculty of Science, Universiti
Teknologi Malaysia, Johor,
Malaysia
2 Centre for Sustainable
Nanomaterials, Ibnu Sina
Institute for Scientific and
Industrial Research, Universiti
Teknologi Malaysia, Johor,
Malaysia
3 School of Marine Science and
Environment, Universiti
Malaysia Terengganu, Kuala
Terengganu, Malaysia
4 Faculty of Applied Sciences,
Universiti Teknologi MARA,
Selangor, Malaysia
5 Department of Chemistry,
Jamia Millia Islamia, Central
University, New Delhi, India
Agarose- and alginate-based biopolymers
for sample preparation: Excellent green
extraction tools for this century
Recently, there has been considerable interest in the use of miniaturized sample preparation
techniques before the chromatographic monitoring of the analytes in unknown complex
compositions. The use of biopolymer-based sorbents in solid-phase microextraction tech-
niques has achieved a good reputation. A great variety of polysaccharides can be extracted
from marine plants or microorganisms. Seaweeds are the major sources of polysaccha-
rides such as alginate, agar, agarose, as well as carrageenans. Agarose and alginate (green
biopolymers) have been manipulated for different microextraction approaches. The present
review is focused on the classification of biopolymer and their applications in multidisci-
plinary research. Besides, efforts have been made to discuss the state-of-the-art of the new
microextraction techniques that utilize commercial biopolymer interfaces such as agarose
in liquid-phase microextraction and solid-phase microextraction.
Keywords: Agarose / Biopolymers / Green chemistry / Sample preparation / Solid-
phase extraction
DOI 10.1002/jssc.201501207

Received October 31, 2015

Revised December 9, 2015
Accepted December 30, 2015
1 Introduction
Green chemistry (sustainable chemistry) is an area of chem-
istry and chemical engineering that strives to design pro-
cesses/products that reduce/eliminate the use and generation
of hazardous materials [1]. Chemists are concerned about the
future of the environment and worried about what will hap-
pen if we continue to suffocate the earth with hazardous sub-
stances in chemical processes. Therefore, it is important to
develop green chemical processes with sustainable develop-
ment practices to eliminate environmental degradation and
pollution.
Conventional extraction methods such as LLE or solvent
extraction involving large amounts of organic solvents are
generating hazardous wastes to the environment, which is
contradicting the concept of green chemistry [2]. To meet
green chemistry requirements, eco-friendly extraction and
Correspondence: Professor Mohd Marsin Sanagi, Department
of Chemistry, Faculty of Science, Universiti Teknologi Malaysia,
81310 UTM Johor Bahru, Johor, Malaysia
E-mail: marsin@kimia.fs.utm.my
Fax: +607-5566162
Abbreviations: AF, agarose film; AFME, impregnated AF mi-
croextraction; AG, agarose gel; HF-LPME, hollow-fiber LPME;
HS, headspace; MWCNT, multiwalled carbon nanotube;
PAH, polycyclic aromatic hydrocarbon; PMMA, poly(methyl
innovations for a cleaner analysis are urged. Corollary, SPME
and LPME have emerged as the latest green analysis to replace
SPE and LLE. These techniques are categorized as “preven-
tion” under the 12 principles of green chemistry proposed by
Anastas and Warner in 1991 [3].
Although green techniques such as SPME and LPME
have been progressively developed and modified, the appli-
cation of the techniques is still confined to research and aca-
demic institutions only. This is mainly because most of the
green techniques were validated in-house. Food manufactur-
ers and private industries are still employing the conventional
techniques, such as LLE. It was declared as standard reference
method by some of the associations who established the max-
imum residue levels of food and environmental pollutants.
Therefore, the publication of the green techniques should be
made available to those associations and the public.
In recent years, great attention has been focused on the
search for an alternative to petroleum-based materials, par-
ticularly from renewable and biodegradable resources. At the
present time, a shift in emphasis in green chemistry is appar-
ent with the desire to develop more environmentally friendly
routes and explore environmentally green solvents and ma-
terials [4–6]. Therefore, the use of less organic solvent and
biodegradable material as extraction tools has formed the
main thrust of today (green extractions). This review focuses
on the classification of biopolymers, outlines their present
applications in multidisciplinary research, and discusses the
state-of-the-art of the new microextraction techniques that
∗ Additional corresponding author: Professor Imran Ali

methacrylate); SBSE, stir bar sorptive extraction E-mail: drimran_ali@yahoo.com


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J. Sep. Sci. 2016, 39, 1152–1159
utilized commercial biopolymer such as agarose in LPME
interfaces and SPME.
2 Biopolymers
Biopolymers or biodegradable polymers can be classified
into four categories, which include those obtained from re-
newable biomass, synthesized microbially, synthesized from
petroleum-based chemicals, and chemically synthesized us-
ing monomers obtained from agro-resources (Fig. 1) [7]. The
first category can be further defined and termed as agro-
polymers, whereas the others are called biopolyesters. Nowa-
days, biopolymers are of interest in multidisciplinary research
as these can be degraded by the living organisms upon dis-
posal, thus, saving disposal and recycling costs.
2.1 Biomass biopolymers
This category consists of animal- and plants-based polysac-
charides, protein and lipids. Agarose and chitin are the most
well-known examples of polysaccharide-based biopolymers
that are frequently utilized in multidisciplinary researches.
Agarose that consists of alternating D-galactose and 3,6-
anhydro-L-galactose, is extracted from seaweed [8]. Agarose
forms gel through aggregating its hexagonal fibers of six dou-
ble helices and imbibing large quantities of water within its
network. Its gel-forming ability, hydrophilic polymeric net-
work, chemical inertness, and flexible pore size have en-
abled its widespread applicability. It is especially popular as
a gel electrophoresis medium [8], pervaporation membrane
for the dehydration of organics [9,10], optical sensor support-
ing material [11, 12], and drugs controlled release agent [13].
Chitin, which consists of 2-acetamino-2-deoxy-␤-D-glucose, is
the supporting material found in crustaceans and insects [14].
Chitin is readily degraded by chitinases that are widely found
in nature such as bacteria, fungi, and plants. It is nontoxic,
antibacterial, hydrophilic, with a gel-forming capacity and
affinity to proteins. It has been widely applied in medical in-
dustry to suppress tumor cells growth and accelerate wound
healing. Besides, it is being used in chemical industry to
isolate lectins, food industry to immobilize enzymes, and
in industrial waste treatment [14]. Chitosan, (poly[1,4-␤-D-
glucopyranosamine]), is a fiber-like substance derived from
chitin by partial alkaline deacetylation process. The most pop-
ular use of chitosan is as a natural sorbent to recover precious
metals [15] and remove toxic metal ions [16]. Gelatin is the
biopolymer of animal-based protein family. Gelatin has been
widely used as delivery vehicle for the controlled release of
bioactive molecules [17] and cathode binder in battery indus-
try [18]. Alginic acid or its salt called alginate is among the
polysaccharides that occur in the cell walls of a large number
of algal species. It is a copolymer consisting of the residues of
␤-1,4-linked D-mannuronic acid (M-block) and ␣-1,4-linked
L-guluronic acid (G-block) [19]. The use of alginate for the
removal of toxic metals as well as for the recovery of precious

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Sample Preparation 1153
metals [20–22] and dyes [23] from aqueous solution has been
extensively studied.
2.2 Microbial production of biopolymers
Poly(hydroxyl-butyrate) is one of the bacterially produced
polyhydroxyalkanoates. Poly(hydroxyl-butyrate) has been
blended with polysaccharide-based biopolymers to enhance
the tensile and tear strengths of polysaccharide-based biopoly-
mers [24]. The blend could be applied as biodegradable plas-
tics, which have a low price as the polysaccharide-based
biopolymers are from renewable resources.
2.3 Petrochemical-based biopolymers
Polycaprolactones, polyesteramides, aliphatic copolyesters,
and aromatic copolyesters belong to this category [7]. Aliphatic
polyesters with reactive functional groups can be prepared by
polycondensation reactions or by ring-opening polymeriza-
tion and cyclic esters. Synthesis of aliphatic polyester by poly-
condensation of diols and dicarboxylic acid can be linked to
Carother’s work in the 1930s. Nowadays, effective techniques
have been developed to prepared high molecular weight
polyesters. For example, poly(g-caprolactone; polycaprolac-
tone) is usually obtained by ring-opening g-caprolactone in
the presence of metal oxide.
2.4 Chemically synthesized agro-based biopolymers
Poly(lactic acid) is aliphatic polyesters produced by fermenta-
tion of sugar feed stocks, which is a renewable resource [25].
It is popular to apply as biocompatible medical device, drug
delivery agent [26], and industrial packaging due to its resis-
tant property to fatty food, high strength, good heat sealability,
and flexible modulus properties [25, 27].
3 Agarose in microextraction techniques
Recently, the use of different types of solvent holders, inter-
faces, and sorbent holders in microextraction techniques is
frequently reported. It is to overcome the solvent dissolution
problem of single drop microextraction [28] and minimize the
use of sorbents in SPE. However, most of the solvent hold-
ers, interfaces, and sorbent holders reported are synthetic
polymers that are nonbiodegradable. These include hollow
fibers (HFs) [29–32], nylon membranes [33], polypropylene
and polyethylene membrane bags [34, 35], PTFE polymeric
membranes [36], and silica monoliths [37]. Therefore, eco-
friendly biopolymers would be a great choice to replace ther-
moplastics. Certainly, these will make a difference in the
environment today and tomorrow.
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1154 M. M. Sanagi et al.
Figure 1. Classification of biodegradable polymers.
3.1 Agarose-film LPME
Agarose-film (AF)-LPME was developed for the extraction
and preconcentration of polycyclic aromatic hydrocarbons
(PAHs) in the environmental water samples [38]. AF was used
as an interface between donor and acceptor phases, which al-
lowed for selective extraction of the analytes under optimum
conditions. AF-LPME device proved to be low-cost and, thus,
reuse or recycle of the film was not required to eliminate the
analytes carryover between runs. In 2012, Sanagi et al. [38] re-
ported AF-LPME system for the extraction of selected PAHs
in water samples. The invented system utilized environment-
friendly biopolymers, agarose for the first time as an LPME

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J. Sep. Sci. 2016, 39, 1152–1159
Figure 2. (A) AF and (B) glass tube
used in AF LPME.
interface in microextraction technique. In this work, a dehy-
drated AF was attached at the end of a tiny glass tube to serve
as a barrier during LPME (Fig. 2). The acceptor solvent was
introduced into the tube and then dipped into the sample
solution for extraction. After extraction for a prescribed time,
the acceptor solvent was withdrawn with a GC microsyringe
and injected into the GC. The film was entitled for single
extraction only to avoid analyte carryover.
In the study, the structured layers of the agarose gel (AG)
stacked to each other to form a thin nanopore film during the
dehydration of the 0.8% w/v AG. The AF serves as a selective
barrier that allows for the diffusion of the analytes, where
its function is similar to the HF that is frequently applied in
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J. Sep. Sci. 2016, 39, 1152–1159
LPME. However, the disadvantage of the AF was its poros-
ity, which was estimated as 39% as compared to HF, which
was about 70% [39, 40]. However, this shortcoming can be
addressed by applying smaller volume of acceptor phase to
increase the analytes enrichment. In comparing AF-LPME
with other reported microextraction techniques, the authors
conluded that the AF-LPME techniques offered better sen-
sitivity as compared to headspace (HS) solvent microextrac-
tion [41] and dynamic LPME [42]. But it achieved compa-
rable sensitivity as dispersive liquid–liquid microextraction
based on the solidification of a floating organic drop [43] and
ultrasound-assisted emulsification microextraction [44]. Stir
bar sorptive extraction (SBSE) [45, 46] appears to provide bet-
ter sensitivity with much longer extraction and desorption
time in comparison to AF-LPME. Although AF-LPME has
merits and demerits of analytical achievements, yet it has
simple procedures. The use of biopolymer is an added incen-
tive as a new microextraction technique for physical barrier
to eliminate sample matrix effect.
3.2 Agarose solvent-impregnated gel LPME
A new microextraction technique termed as AG-LPME was
developed for the extraction of PAHs in water [47]. Due to
the hydrophilic properties of agarose, the selectivity of AG-
LPME was evaluated on hydrophilic triazine herbicides. The
AG-LPME showed significantly higher extraction efficiencies
as compared to HF-LPME. The method offered superior en-
richment factors of up to 300, and trace LODs in the range
of 0.02–0.04 ␮g/L. Loh et al. [47] applied AG as a solvent
holder in LPME for the first time, which was termed as
solvent-impregnated AG-LPME. The technique shares the
same practical principle as solvent-impregnated resin [48–60]
extraction, and LPME that utilized knitting wool as solvent
holder [61]. These techniques have been extensively applied
as a sample preparation tool to extract trace metals [48–54]
and organic compounds [55–60] from environmental sam-
ples. The solvent was immobilized within the resin or sol-
vent holder to function as an extractant. These approaches
can withstand even high agitation speeds and long extraction
times to enhance analytes mass transfer without the solvent
dissolution problem. The only difference between the AG-
LPME and the mentioned techniques is the solvent holder
applied in the AG-LPME, a green biodegradable biopolymer.
The technique combines both microextraction format and
green material as extraction tools. These have great contribu-
tion to support the green analytical chemistry.
For the preparation of solvent-impregnated AG, the au-
thors exchanged the solvent in the AG from water to ethanol
and then subsequently to 1-octanol through diffusion. The
solvent exchange process, especially the exchange from wa-
ter to ethanol, was carried out using increasing percentage
of ethanol to avoid the agarose framework from collapsing
(Fig. 3). The extractant-impregnated agarose disc was then
tumbled into the sample solution for extraction. After the ex-
traction for a prescribed time, the agarose disc was removed

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Sample Preparation 1155
and centrifuged to squeeze out the solvent. The supernatant
was then injected into the GC–MS system.
In the same article, the authors compared the analytical
performances of AG-LPME, HF-LPME, and AF-LPME un-
der their respective optimum conditions for the extraction of
selected polycylic PAHs using the same amount of extrac-
tant. The report revealed that the extraction efficiencies of
AG-LPME were comparable to those of the HF-LPME. But
both techniques were superior as compared to the AF-LPME.
The authors then concluded lower extraction efficiency of AF-
LPME. It was mainly due to the limited surface area of film,
smaller pore diameter, and low porosity. Sanagi et al. [62]
compared the analytical performances of AG-LPME and HF-
LPME for the extraction of selected triazine compounds in
water. The paper revealed that the extraction efficiencies of
AG-LPME were superior as compared to HF-LPME for the
extraction of hydrophilic compounds (except for the atrazine).
This finding was opposing to the comparison made for the ex-
traction of nonpolar compounds conducted by Loh et al. [47].
The authors concluded that the hydrophilic nature of agarose
prioritized the partitioning of polar compounds. This prop-
erty has been the major incentive to agarose when it is applied
as solvent holder, as compared to nonbiodegradable and hy-
drophobic polypropylene HF.
3.3 Agarose multiwalled carbon
nanotube-impregnated film microextraction
After the development of AF-LPME system, Loh et al. [63]
modified AF-LPME by agarose-immobilized multiwalled car-
bon nanotubes (MWCNTs) within the mesoporous film in
SPME. The technique was named as MWCNT-impregnated
AF microextraction (MWCNT-AFME). It was applied to
the analysis of selected PAHs in green tea beverage. The
procedure involved the use of circular-shaped MWCNT-
impregnated AF pierced with a needle. It was dipped into
sample solution for the extraction at a prescribed time.
The sorbent was then sonicated to desorb the analytes be-
fore ␮-HPLC analysis. This innovation permitted the use
of biodegradable biopolymer to serve as sorbent holder in
SPME, which then eliminated the use of plasticizer or ther-
moplastic as sorbent holder. The authors concluded that the
MWCNT-AFME was equally sensitive as SPE [64], LLE [65],
SBSE [66], and HS-SPME [67] for the extraction and determi-
nation of PAHs from tea samples. The minimal amounts of
MWCNTs were distributed evenly within the AF. These have
greatly enhanced the contact among analytes and sorbents.
This approach has resulted in shorter extraction time as com-
pared to SBSE and HS-SPME. In addition, the simplified pro-
cedures and apparatus, and utilization of green biopolymer,
have been the added advantages to MWCNT-AFME.
Poly(methyl methacrylate) (PMMA)-grafted agarose
was successfully prepared in our laboratory with ceric
ammonium nitrate as the radical initiator. The grafted
copolymer was evaluated and used successfully as the
sorbent in ␮-SPE for the extraction and preconcentration of
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1156 M. M. Sanagi et al.
selected organophosphorus pesticides in water. In general,
the new method proved to be efficient, simple, rapid, and
supportive toward the green chemistry concept.
3.4 Agarose-grafted PMMA
In the last decade, there has been increasing interest in
the modification of low-cost natural polysaccharides as ad-
sorbents by grafting with synthetic polymers. These mate-
rials (grafted biopolymer) have been applied as adsorbents
to extract trace metals [68], dyes from environmental sam-
ples [69–71], drug delivery [72, 73], and flocculant [74, 75]. Re-
cently, Pourmand et al. [76] prepared a new grafted copolymer
with agarose for dispersive ␮-SPE and the preconcentration of
selected heavy metal ions [Cd(II), Ni(II), Cu(II), and Zn(II)] in
vegetable and water samples. The developed system utilized
environmentally friendly biopolymer (agarose) for the first
time in dispersive ␮-SPE technique. In this study, agarose
was grafted with PMMA by microwave-assisted free radical
polymerization combined with ceric ammonium nitrate as
the radical initiator.
3.5 Sodium alginate-grafted PMMA
Recently, modified biopolymers (polysaccharides) have re-
ceived much attention as low-cost adsorbents for the removal
of pollutants in water. High selectivities toward aromatic com-
pounds and metals were observed because of their unique
physicochemical properties. These are due to the presence
of various functional groups in the polymer chains [77]. It
is important to mention here that grafting is one of the
convenient methods among the methods of modification of
biopolymers [78]. The graft copolymerization is an attractive
method to introduce a variety of functional groups to main
polymer backbone. The grafting of synthetic polymer onto
biopolymer backbone yields a hybrid material with a wide
range of properties. It could be tailored to many applications

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J. Sep. Sci. 2016, 39, 1152–1159
Figure 3. (A) AG disc and (B) AG
discs dipped in 70% ethanol so-
lution.
in diverse areas. Radicals can be generated along polysaccha-
rides main chains in the presence of chemical initiators or by
applying irradiation and addition of vinyl monomers yields
polysaccharide-graft copolymer through “grafting from” free
radical polymerization.
Many researchers have reported the feasibility of using
calcium alginate beads as low-cost adsorbent for the removal
of pollutants in water, particularly heavy metals [79–82]. One
way to improve the mechanical strength as well as adsorption
capacity of sodium alginate is by graft copolymerization with
vinyl monomers. Salisu et al. [83] have documented stud-
ies on chemically induced graft copolymerization of vinyl
monomers onto sodium alginate and their potential appli-
cation in diverse areas. Recently, Salisu et al. [84] prepared
PMMA graft sodium alginate by radical polymerization us-
ing benzoyl peroxide as initiator. The product was further
cross-linked to form beads. The developed beads showed high
adsorption capacity for lead ions from aqueous solutions. In-
terestingly, these beads could be regenerated by dilute nitric
acid for repeated usages.
3.6 Agarose/chitosan reinforced and blended
MWCNT microextraction
Apart from chemical modifications, noncovalent interactions
offer simple and effective modifications to meet the require-
ments for practical applications. Noncovalent interactions
are promising to improve polysaccharides properties and
compatibility, and ensure long-term stability while retaining
their great original properties [85, 86]. It is important to un-
derstand direction of polymer self-assembly to utilize these
interactions. The most used noncovalent interactions are
blending, layer-by-layer self-assembly, electrochemical sur-
face deposition, and cross-linking. Recently, Wan Ibrahim
et al. [87] successfully synthesized and characterized the
MWCNTs reinforced blended agarose/chitosan composite
film. The study revealed that reinforcement of MWCNTs into
agarose/chitosan-blended film by physical solutions method
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J. Sep. Sci. 2016, 39, 1152–1159 Sample Preparation 1157

Table 1. Selected applications of agarose- and alginate-related materials in extraction

Number Analytes Matrices Techniquesa) Limit of detection Reference

1 Polycylic PAHs Environmental water AF-LPME 0.01–0.04 ␮g/L [28]

2 Polycylic PAHs Drinking water AG-LPME 9–14 ng/L [37]
3 Polycylic PAHs Green tea beverage MWCNT-AFME 0.1–50 ng/L [53]
4 Triazine herbicides Drinking and environmental water AG-LPME 0.02–0.04 ␮g/L [52]
5 Cadmium, nickel, copper, zinc Vegetables and natural water A-g-␮SPE 0.6–1.8 ng/L [66]
6 Lead Water samples Alg-g-␮SPE – [74]
7 Methylene blue Water samples Adsorption – [79]
8 Methylene blue Water samples Adsorption – [80]
9 Nickel Table salt and baking soda SPE 0.49 ␮g/L [81]
10 Tricyclic antidepressants Tap water and human urine EME 0.02–0.2 ␮g/L [85]
11 Triazine herbicides Water samples MWCNTs-AG-␮SPE 0.32–0.34 ␮g/L [86]

a) A-g-␮SPE, agarose-grafted PMMA ␮SPE; Alg-g-␮SPE, alginate-grafted PMMA ␮SPE; EME, electro-driven membrane extraction.

showed good dispersion of MWCNTs and highly compati- 5 Conclusions

ble blend. Native ligand with electron donor groups (–NH2 )
on chitosan made it a highly potential dispersion agent for
MWCNTs and prevented deactivation of sorbent by agglom-
eration [63, 88].The performance of synthesized composite
film was evaluated in ␮-SPE for selected nonsteroidal anti-
inflammatory drugs and tricyclic antidepressant drugs. Four
stacked pieces (5.0 × 5.0 mm2 ) pierced by a syringe needle
were required for each extraction.
4 Challenges and future perspectives
Of course, polysaccharide-based sorbents are ideal for green
technology. The polysaccharides such as agarose, alginate,
amylose, cellulose, curdlan, chitosan, xylan, dextran, and in-
ulin may be used as sorbents. There is a big problem in
using these molecules due to their hydrophilic nature. They
get swollen in aqueous media and hence, need derivatization.
Sometimes, derivatization is a challenging job due to extreme
reaction conditions and use of costly and hazardous solvents.
Therefore, these are the big hurdles for making these sor-
bents as green and inexpensive ones.
The above-mentioned problems can be solved by de-
veloping innovative derivatization protocols. Besides, low-
molecular-weight polymers may be handled easily in com-
parison to giant molecules. Therefore, the selection of the
sorbent should be executed carefully. Really, the proper man-
ufacturing of polysaccharide-based sorbents may be boon to-
ward green and inexpensive sample preparation technology.
Besides, these sorbents may be helpful to solve the real-life
water pollution problems globally. Moreover, these polymers
are chiral in nature and may be used to extract enantiomers
selectively in sample preparation. There is no paper on this
issue using polysaccharide polymers. This will be new and in-
novative sample preparation method for enantiomeric analy-
ses in unknown matrices. The future of these sorbents seems
to be quite bright. Hopefully by the middle of this century,
the polysaccharide-based sorbents will be preferred choice of
the green chemists and technologists.
During the write up of this article, it was observed that re-
search on adsorbent is progressive from nonbiodegradable
materials to biodegradable ones. In this direction, agarose
polysaccharide has been used by some workers. Native
agarose and sodium alginate along with its impregnation and
blending as well as grafting and cross-linking have been used
for sample preparation and water treatment (Table 1). Other
agarose and sodium alginate-based material applications in-
clude adsorption of methylene blue [89, 90] preconcentration
of nickel in table salt and baking soda [91], agarose-cytosine
as sensor [92], cation exchangers and protein adsorption [93],
fluorescent polymeric material [94], alternative interfaces for
micro electrodriven membrane extraction [95], and determi-
nation of triazine herbicides [96]. These approaches seem to
be innovative as having green chemistry approach. Besides,
polysaccharide is available in plenty in nature and, hence,
these sorbents may be inexpensive. It has been observed that
agarose-based sorbents are limited to research and develop-
ment only. Therefore, there is great need to use them in
solving real-life problems. We hope that the middle of this
century may be of biodegradable green adsorbents.
The authors would like to thank Universiti Teknologi
Malaysia for facilitations and the Ministry of Education
Malaysia for financial supports through research Grant Num-
ber QJ130000.2526.03H79.
The authors have declared no conflict of interest.
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