International Journal of Biological Macromolecules 309 (2025) 143173

Contents lists available at ScienceDirect

International Journal of Biological Macromolecules

journal homepage: www.elsevier.com/locate/ijbiomac

Review

Chitosan-based adsorbents for wastewater treatment: A

comprehensive review
Franciele da Silva Bruckmann a , Janaína Oliveira Gonçalves b, Luis Felipe Oliveira Silva b,* ,
Marcos Leandro Silva Oliveira b, Guilherme Luiz Dotto a,* , Cristiano Rodrigo Bohn Rhoden c,*
a
Research Group on Adsorptive and Catalytic Process Engineering (ENGEPAC), Federal University of Santa Maria, Av. Roraima, 1000-7, Santa Maria, RS 97105–900,
Brazil
b
Department of Civil and Environmental, Universidad de la Costa, Calle 58 #55-66, 080002 Barranquilla, Atlántico, Colombia
c
Laboratório de Materiais Magnéticos Nanoestruturados – LaMMaN, Universidade Franciscana – UFN, 97010-032, Brazil

A R T I C L E I N F O A B S T R A C T

Keywords: Chitosan has emerged as a promising biopolymer for developing eco-friendly adsorbents for wastewater treat­
Adsorption ment contaminated by different compounds, such as heavy metals, pharmaceutical compounds, pesticides, and
Emerging pollutants synthetic dyes. Despite its biocompatibility and biodegradability, the application of pristine chitosan in
Non-conventional adsorbents
adsorption systems is limited by its low surface area, poor thermal and mechanical stability, and high solubility
Chitosan
under acidic conditions. This comprehensive review analyzes recent advances in chitosan’s chemical and
physical modification to enhance its physicochemical, morphological, and adsorption performance. The role of
crosslinking agents, nanocomposite synthesis, and the incorporation of magnetic particles in improving the
material’s textural characteristics, selectivity, and regeneration potential was highlighted. The novelty of this
work lies in its evaluation of how these structural modifications can influence the adsorption mechanisms and
performance in different classes of contaminants under varying experimental conditions. Furthermore, this re­
view highlighted the importance of structural-functional correlations, including surface area, pore distribution,
crystallinity, and thermal stability, in optimizing adsorbents’ adsorption capacity and reusability. The study also
provides critical insights into the effects of pH, temperature, ionic strength, and competitive adsorption in
multicomponent systems, furnishing valuable details about the design of high-performance and sustainable
chitosan-based adsorbents.

1. Introduction systems, including adsorption [10], oxidation [11], coagulation-

flocculation and flotation [12], and photocatalysis [13].
Many chemical compounds are classified as emerging pollutants, Adsorption is a mass transfer process and surface phenomenon be­
such as heavy metals, pesticides, organic dyes, pharmaceuticals, and tween a liquid or gas phase and to solid material. The effectiveness of the
personal care products [1–3]. Water contamination results from process and degree of interaction between adsorbent and adsorbate
anthropogenic activity related to industrial processes, agrochemicals, depends on various factors such as temperature, contact time, concen­
domestic and hospital sewage, and the unsuitable disposal of drugs tration, affinity by the contaminant, and chemical composition of the
[4,5]. adsorbent material [14–17]. This tertiary process is commonly explored
Environmental contamination by emerging pollutants is a global for water remediation due to its excellent performance in removing
problem due to their bioaccumulation, persistence, low degradability, microcontaminants without generating by-products, low energy de­
and numerous negative effects on aquatic life, microbiota, animals, and mand, feasibility, and ease of operation [4,18].
human health [6,7]. However, many of these compounds must be fully Chitosan (CS) is a heteropolysaccharide (poly-β-(1-4)-2-amino-2-
removed from wastewater treatment systems due to low concentration deoxy-D-glucose) derived from the deacetylation of chitin with a poly­
(ng L− 1), complex chemical structure, and hydrosolubility [8,9]. In this meric chain such as cellulose [19,20]. The CS polymer is considered eco-
scenario, a set of techniques has been used in wastewater treatment friendly due to its low toxicity and good degradability, which turns a

* Corresponding authors.
E-mail addresses: [email protected] (L.F.O. Silva), [email protected] (G.L. Dotto), [email protected] (C.R.B. Rhoden).

https://doi.org/10.1016/j.ijbiomac.2025.143173
Received 4 August 2023; Received in revised form 11 April 2025; Accepted 13 April 2025
Available online 15 April 2025
0141-8130/© 2025 Elsevier B.V. All rights are reserved, including those for text and data mining, AI training, and similar technologies.
F. da Silva Bruckmann et al. International Journal of Biological Macromolecules 309 (2025) 143173

promisor adsorbent material [21]. However, this biopolymer exhibits compounds are used in diverse applications such as electroplating,
some properties, such as low specific surface area, weak thermal and firefighting foam, and sulfluramide production in China. In 2006, China
mechanical stability, and easily soluble in acidic conditions due to the exported approximately 100 tons of PFOS to Brazil, the European Union,
protonation of amino groups, restricting its application as an adsorbent and Japan, as reported by the Ministry of Environmental Protection of
in a wide pH range [21–23]. Furthermore, another drawback of chitosan China [45–47]. The Stockholm Convention established measures to
and other conventional materials is the recovery of the aqueous solution eliminate or restrict the release of persistent organic pollutants (POPs),
after the adsorption process [24–26]. listing industrial organic compounds and pesticides, including the
Recently, several trends have emerged in using chitosan in waste­ original 12 POPs. Since then, the list of POPs has been regularly updated
water treatment systems through chemical modification of its during conferences of the participating parties, with new compounds
biopolymer structure and the development of chitosan-based nano­ being added. Following the Conference of the Parties (COP) held in
composites. These tendencies reflect the growing interest in using chi­ Switzerland in 2019, the list now includes 27 POPs [48]. In aquatic
tosan and its derivatives as sustainable and effective solutions in environments, they are highly toxic and have a great capacity for
wastewater treatment, aiming to overcome the limitations related to the “bioaccumulation” in living organisms, as they are dissolved in the tis­
biopolymer and increase selectivity for certain contaminants [27–29]. sues of living beings or organic matter.
The economic feasibility, abundance, and chemical reactivity of Concerning synthetic organic dyes, the growing population led to the
functional groups allow the development of chitosan-based adsorbents. need to increase the production of food, cosmetics, drugs, and other
In this way, diverse chemical modifications have been developed to products to satisfy the basic demands of everyday life [49]. Global
improve the physicochemical stability, limitations associated with the production of synthetic dyes is estimated at around 700 thousand tons
process and the textural properties, and easy recyclability that are annually. Between 10 % and 20 % of these dyes are lost during
extremely important in the adsorption process [30,31]. Among these, manufacturing, resulting in their presence in industrial effluents [50].
magnetic chitosan composites stand out due to their ease of separation Therefore, organic dyes contribute to aquatic contamination since many
via magnetic fields, high adsorption efficiency, and potential for reuse, of these compounds have low degradability and high stability [51].
making them particularly attractive for practical wastewater treatment Considering the high stability and aqueous solubility of dyes, diverse
applications. Approaches include the synthesis of nanocomposites using negative impacts on the environment are observed, such as a decrease in
nanodiamond [32], cross-linking reactions with ethylenediaminetetra­ the photosynthesis process and oxygen levels alteration of the produc­
acetic acid, polyethylene glycol diglycidyl ether, and glutaraldehyde tion of chlorophyll, carotenoids, and protein contents [52,53].
[32–34], oxidation reaction [35], and magnetic adsorbents [30,36–38]. Furthermore, chronic toxicity was also observed in crustaceous (Daphnia
Although numerous review studies on the use of chitosan as an magna) exposed to different dyes [54]. However, dyes have been
adsorbent material have been published in recent years, the current considered hazardous chemicals and intermediate products generated
work has focused on detailing the influence of chemical modifications in after effluent treatment [55]. A decrease in survival, malformation,
its biopolymeric matrix and adsorbent properties on the adsorption degeneration, and DNA damage in Danio rerio was observed during the
performance of various contaminants, such as pharmaceutical com­ embryonic and larval stages e when exposed to Maxilon Blue 5G and
pounds, pesticides, dyes, and heavy metals. For better understanding, Reactive Blue 203 [56].
this review has been divided into the following sections: i: Firstly, in­ Drugs and hormones are also included in the emerging contaminant
sights about the environmental toxicity and impact on human health class because they can bioaccumulate and induce potential toxic effects
caused by the emerging pollutants are reported. ii: The effect of chem­ [57]. Incomplete biotransformation by the organism results in the
ical modifications on chitosan-based adsorbents was discussed, high­ excretion of the unchanged form of the compounds in urine and feces
lighting the particularities and characteristics. iii: After was provided [58]. Meantime, synthetic hormones and other substances such as pes­
with comprehensive information about using chitosan-based adsorbent ticides, aromatic organic compounds, and personal care products also
to remove different emerging pollutants, understanding the effects of cause side effects on humans and animals. Due to the capacity to mimic
textural properties of adsorbent, and experimental conditions in the functions, these pollutants modulate the action of endocrine hormones
adsorption behavior. by blocking the synthesis, binding with receptors, and changing hor­
mone levels [59,60]. Teratogenic effects and changes in the swimming
2. Impact on human health and the environment by organic and behavior of the species Xenopus laevis larvae were observed after contact
inorganic pollutants with bisphenol A [61]. Exposure to agrochemical compounds has been
associated with cancer, genotoxicity, and neurological problems [62].
Organic and inorganic compounds have been associated with
developing diverse toxic effects in humans and animals and environ­ 3. Chitosan adsorbent and its modification
mental damage. These pollutants in determined concentrations can alter
homeostasis, producing cytotoxic, genotoxic, and carcinogenic effects Modifications to chemical and physical chitosan are pivotal in
[1,39]. Heavy metals contaminate soils and drinking water through the enhancing the adsorption process. One notable advantage of chemically
wastewater effluents of the industrial sector. On the other hand, the modifying chitosan in adsorption is improving its selectivity. Intro­
toxicity to human health is associated with the ingestion [40–42]. ducing specific functional groups makes it possible to adjust chitosan’s
Although some heavy metals are essential for metabolic and physiologic affinity for certain pollutants, making it more selective for target sub­
functions, this metal class interacts with vital substances such as pro­ stances and reducing the removal of desired components. Furthermore,
teins, DNA molecules, enzymes, and cellular components, modulating chemical modification extends the pH range in which chitosan can be
biochemical processes, and normal organism functions [43,44]. more effective as an adsorbent [63,64]. Physical modification may
Perfluoroalkyl substances were initially produced in 1949 by 3 M involve alterations in chitosan’s morphology and structure. These
Company®, and thousands of tons were manufactured for various ap­ modifications can result in a larger surface area, providing more active
plications over the subsequent decades. In 2000, 3 M, the leading global sites for adsorbent-pollutant interactions. Therefore, it directly con­
producer of PFASs, ceased the production of perfluorinated compounds tributes to an increase in the adsorption capacity of chitosan [65].
and derivatives, which accounted for 95 % of the company’s fluorinated The flexibility of chitosan through chemical and physical modifica­
chemical production. This decision was followed by other companies tions not only optimizes its intrinsic properties but also adapts its
worldwide. However, in 2002, China initiated large-scale production of characteristics to the specific needs of each pollutant. As a result,
PFOS, reaching 246.88 tons in 2006. Due to international environmental modified chitosan becomes a versatile and effective tool in various
policies, production was reduced to 100 tons in 2008. Currently, these contexts, ranging from water treatment to complex industrial processes.

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It is a valuable contribution to efficiently removing pollutants [66]. patterns). The insertion of functional groups in the structure of materials
causes a change in the distance (nm), which XRD diffractograms can
3.1. Influence of chemical modification on the crystallinity of observe. In addition, this measure is used to verify particle agglomera­
nanocomposites tion [69]. A slight shift in XRD patterns can result in partial intercalation
of the compound due to its chemical configuration [70]. Verma et al.
The cross-linking agents are used for enhancing physicochemical [71] observed that the amination reaction is the reason for the absence
stability and thermal properties. The chemical modification/incorpo­ of an XRD pattern at 19.51◦ in the diffractogram of the synthesized
ration methods can reduce the crystalline phases of compounds by composite (Fig. 1).
deposition into the surface and binding with functional groups.
Recently, Xu et al. [67] reported a decrease in magnetite crystallinity 3.2. Effect of chemical modification on textural properties
after modification with chitosan. However, modification of Fe3O4-CS
with MXenes (2D inorganic compounds) reduced agglomeration and Activation of polymers by inserting functional groups enhances their
improved the surface area of the nano adsorbent. versatility and adsorptive capacity. Imidazole and thiazole compounds
Different chitosan contents in nanocomposites also cause a decrease were incorporated into chitosan magnetic microparticles using
in the crystalline peaks, referring to the CuFe-layered double hydrox­ epichlorohydrin as a crosslinking agent, though no significant differ­
ides. Porous interfaces and rough surfaces combined with high crystal­ ences in textural properties were observed [72].
linity contribute by improving in adsorption efficiency of dyes [68]. Another cross-linking reagent employed in inserting more reactive
Similarly, chitosan-based magnetic nanocomposites synthesized by [9] groups into compounds is glutaraldehyde. A typical cross-linking reac­
presented a suppression of crystalline phases assigned to chitosan by tion synthesized The EDTA-functionalized β-cyclodextrin-chitosan
magnetic nanoparticle incorporation on its polymer matrix. Thus, the composite [71]. The chemical reaction resulted in synthesizing the
phases observed in the diffractogram were those related to iron oxide composite with an adsorption/desorption isotherm of the H3 hysteresis
nanoparticles at 2θ ≈ 30.37◦ , 35.42◦ , 43.15◦ , 57.06◦ , and 62.59◦ . loop type, which suggests the existence of mesoporous. Although the
The interlayer size is a parameter employed to verify the influence of adsorbent has a low specific surface area (2.404 m2 g− 1), this parameter
functionalization/modification in the characteristic peaks (XRD may not significantly affect the adsorption efficiency. The influence of

Fig. 1. Influence of chemical modification on the crystallinity of nanocomposites.

Reproduced from: a) [69] Copyrights 2022, Elsevier; b) [68] Copyrights 2022, Elsevier; c) [67] Copyrights 2022, Elsevier; d) [71] Copyrights 2021, American
Chemical Society.

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the textural properties and other experimental conditions on the polymerization reactions, and covalent and supramolecular crosslinking
adsorption performance will be discussed in the next section. can be excellent tools for preventing damage to the polymeric structure
Isotherms and hysteresis loop types are used to determine the char­ [15,87,88].
acteristics of adsorbent material [7]. The isotherms can be present in Recently, Sadiq et al. [88] reported the preparation of magnetic
different geometries according to the porous or absent characteristics. chitosan modified with eutectic solvents. According to mentioned, the
Through the isotherm type and pore size, materials are classified as absence of endothermic and exothermic peaks suggests the high stability
microporous (Dp < 2 nm), mesoporous (2 < Dp < 50 nm), or macro­ of nanoparticles caused by the interaction between amine groups and
porous (Dp > 50 nm) [9,73]. Fe2O3. The in-situ polymerization reaction with polypyrrole improved
Diverse materials such as titanium and iron have been used to the thermal stability of the magnetic composite (γ-Fe2O3-Chitosan). The
enhance chitosan’s performance as an adsorbent. The synthesis of chi­ magnetic compound without the polypyrrole had a first mass loss stage
tosan beads modified with TiO2 and FeO nanoparticles using the ionic at 29 ◦ C, but the hybrid composite suffered the first step at 124 ◦ C [79].
cross-linking method furnishes an adsorbent with a rough and high Magnetization facilitates the separation and recovery of the adsorbent
surface area compared to pristine chitosan (Ch-0.7 m2 g− 1 and Ch-FeO/ from aqueous media after use by applying an external magnetic field,
TiO2-27.1 m2 g− 1) with the presence of micropores [74]. On the other making the process more efficient, reusable, and, therefore, more suit­
hand, a method explored for obtaining adsorbents with excellent per­ able for large-scale applications.
formance and high adsorption capacity is Layered Double Hydroxide The modification of chitosan with carbon nanotubes and polyhedral
(LDH) [75]. oligomeric silsesquioxane enhanced the thermal stability of the
Nanoparticles’ incorporation into the surface of other compounds biopolymer. Afterward, at the temperature of 200 ◦ C, the nano­
can modify textural properties such as surface area, number, and size of composite’s degradation occurs more slowly than pure CS [89]. Carbon
pores [76–78]. Chitosan nanocomposites based on magnetic nano­ nanotube-grafted chitosan presents lower thermal stability than pure
particles were synthesized by a co-precipitation method followed by a chitosan [21].
polymerization reaction to introduce polypyrrole chains on the polymer
surface. The material exhibited different textural properties after the 3.5. Magnetic nanoparticles for incorporation into chitosan surface
polypyrrole was grown between magnetic chitosan porous [79]. Pa­
rameters such as the ball milling time and oxidant type also affected the Different methods are employed to prepare magnetic nanoparticles.
specific surface area of chitosan and its derivatives [35]. The iron salts used in co-precipitation reactions are commonly FeCl3 and
FeCl2 (2:1 M ratio). However, the literature has reported adapted
3.3. Effect of chemical modification on the morphological characteristics methodologies that employ ferrous sulfate (FeSO4) [67,90] in different
of adsorbents proportions (Fe3+: Fe2+) [16], as well as only iron sources [19,76].
In addition, it was possible to verify that the size is quite heteroge­
The composites are multiphasic materials formed by a continuous neous, and particles exhibit morphology predominantly spherical. The
phase (matrix) and dispersed phase (reinforcement). These materials morphology is related to controlled conditions such as temperature,
can be classified into polymeric, ceramic, and metallic [80,81]. Thus, inert atmosphere, and constant stirring [91]. This characteristic also
adsorbents based on composites may exhibit different morphologies, depends on functionalization/modification techniques that can alter the
shapes, and sizes. The morphological characteristics of the adsorbent surface chemistry, resulting in particles with high surface energy (Van
may be involved with the specific surface area and relate to the affinity der Waals forces), a phenomenon that causes agglomeration of particles
for the adsorbate [82]. and a decrease in the specific surface area [92,93]. Furthermore, syn­
Saranya et al. [83] reported the synthesis of composite containing thesizing composites can modify the crystalline phases of start materials,
nanorods of chitosan with a rough surface and numerous pores, which resulting in an adsorbent with an amorphous structure [94].
contribute to the high adsorption performance of heavy metals. Simi­ The incorporation of magnetic particles in compounds that do not
larly, Jin et al. [4] prepared a highly porous chitosan-derived adsorbent show magnetic behavior can many cases, result in compounds with low
with large channels containing mesopores (2–8 nm) and a higher surface saturation magnetization (Ms) values [9,95]. The lower values for the Ms
area than pure chitosan. Wang et al. [84] studied the synthesis of compared to pure magnetite can also be attributed to the surface effects,
magnetite-functionalized chitosan employing the crosslinking tech­ a decrease in size, and an agglomeration of particles. The hysteresis
nique. The incorporation in the chitosan matrix promotes the prepara­ loops type S are characteristic of particles with superparamagnetic
tion of nanoparticles with quasi-spherical morphology with some properties [18,30,95]. Tang et al. [3] synthesized nitrilotriacetic acid-
aggregates. modified magnetic chitosan-based microspheres through the cross-ling
The different contents of chitosan used in the reaction changed the reaction using glutaraldehyde. As expected, magnetic adsorbent pre­
morphology of the nanocomposite. While low amounts of biopolymer sented a lower saturation magnetization value (21.6 emu g− 1) than
are related to a rough and porous surface, a high percentage of chitosan pristine Fe3O4 (84.94 emu g− 1). Magnetic chitosan hydrogel beads
resulted in a smooth and homogeneous material [68]. The chitosan- modified by cross-linking method with isophthalic-dichloride also pre­
based adsorbent with a homogeneous surface was also reported by sented similar magnetic behavior after the cross-linkage procedure,
[77]. The chitosan and hydrocalumite composite presented a smooth which indicates that the magnetic composites showed lower Ms values
morphology before adsorption. However, after chromium removal, the than pure magnetic nanoparticles [30]. These modifications improve the
material exhibited a rough characteristic, supporting that the presence physicochemical properties of chitosan and expand its applicability in
of the adsorbate caused the structural changes. removing a broad spectrum of pollutants commonly found in industrial
and municipal wastewater.
3.4. Thermal stability of chitosan-based adsorbents As summarized in Table S1, it was possible to observe that the unique
characteristics and properties were acquired by modifying the polymeric
Thermal analysis is a set of techniques used to predict the stability, structure. These composites presented different sizes, shapes, and
decomposition, and impurities of compounds at a given temperature and physicochemical, thermal, and textural properties that can furnish
the residual water present in the sample. Chitosan is a natural excellent characteristics as the adsorbent material in removing several
biopolymer with excellent properties and high thermal stability emerging microcontaminants, which will be covered in the following
(~280 ◦ C) [85]. The temperature can alter the characteristics of the topic.
polymer, such as the mechanical resistance, solubility, and rheological Composite materials are produced to reduce the limitations and
properties [86]. Thus, the ionic gelation (polyelectrolytes), investigate the synergic effects in an adsorption process. As reported, the

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association of one or more compounds can improve the various char­ chitosan films of different sizes using glutaraldehyde (3 %) at room
acteristics of conventional materials. The limitations associated with the temperature.
adsorption are the high cost of obtaining adsorbents, the difficulty of Another strategic approach to improve the chitosan performance as
aqueous medium separation, easy water solubility, low stability to the adsorbent material was recently reported by Rahmi et al. [33].
variations of pH, and mainly, the recyclability and reuse of the adsor­ Magnetic adsorbent-based chitosan was synthesized by a crosslinking
bent material [9,96,97]. Thus, numerous efforts have been made to reaction using polyethylene glycol diglycidyl ether (PEGDE). The mag­
develop efficient, eco-friendly adsorbents with higher stability and netic adsorbent material exhibited a high intensity in the absorption
excellent cost-effectiveness [9,19]. band related to hydroxyl groups after the cross-linkage. Also, the ma­
Regarding chitosan, the high solubility in the acid medium (pKa = terial presented an expressive band at 582 cm− 1 assigned to Fe–O
6.5) decreases its use as an adsorbent due to the narrow pH range [98]. stretching vibration, confirming the incorporation of magnetic nano­
The protonation of amine groups (NH2) causes an electrostatic repulsion particles on the polymer structure. Similarly, a combined crosslinking
between polymer chains, resulting in the solvation of chitosan molecules reaction using ethylenediaminetetraacetic acid (EDTA) and PEGDE was
(Fig. 2) [99,100]. employed to modify the chitosan. The outcomes of this study showed
Although the high solubility of chitosan is still a limitation for that the EDTA contents affected the crystallinity patterns of chitosan due
employment as an adsorbent, this characteristic allows the chemical/ to intramolecular hydrogen bonds. Also, the amount of EDTA influenced
physical modification of structure, which improves the physicochemical the methylene blue adsorption, showing the important role of amine
properties of chitosan-based composites and produces porous and dense functional groups on pollutant uptake.
polymeric structures [6]. Improve these properties, and crosslinking Also, the amount of EDTA influenced the methylene blue adsorption,
reactions are commonly used to modify the polymer chain. Crosslinking showing the important role of amine functional groups on pollutant
reactions occur by distinct reactional mechanisms that include covalent, uptake.
polyanionic, hydrogen, and hydrophobic interactions and physical in­ As discussed throughout this section, the various physical and
teractions [69,101,102]. chemical modifications applied to chitosan show that tailoring chitosan-
The covalent interactions generally involve the nucleophilic addition based materials enhances their performance as adsorbents. Improving
between NH2 groups (chitosan) and carbonylic compounds (crosslinking porosity, surface area, and functional group availability enhances the
agent), resulting in the formation of a Schiff base [103]. Polyanionic material’s interaction with different pollutants. Therefore, the next
agents modify the chemical structure through electrostatic reactions section explores how these modified chitosan-based materials perform
[83,104]. Among the polyanions, sodium tripolyphosphate (TPP) is the in adsorption processes, highlighting the key factors influencing their
reagent most employed to synthesize chitosan nanoparticles by ionic efficiency in removing emerging contaminants.
gelation [99].
The glutaraldehyde (GLU) is by far the most agent crosslinking used 4. Adsorption process
to modify the structure of the chitosan [64,105–107]. Numerous works
reported the employment of reagents at different concentrations and In the batch adsorption mode, the different experimental conditions
under reactional conditions. Figueiredo Neves et al. [24] synthesized a tested may interfere with the efficiency of the adsorption process. These
magnetic chitosan/quaternary ammonium-salt/graphene oxide com­ effects can be observed by changing the surface charge of the adsor­
posite for application as the adsorbent of organic dyes. The crosslinking bents, ionization of the functional groups of chemical compounds,
reaction was conducted under mild conditions, using only 3 mL of GLU reduction of kinetic energy, competition for active sites, and electro­
solution (50 %) and sodium hydroxide (1.0 mol L− 1) to prepare azo­ static repulsion [25,109]. Thus, this section discusses the influence of
methine. Similarly, Wang et al. [84] developed a system for obtaining several experimental parameters on the adsorption phenomenon.
magnetic chitosan nanoparticles using reverse-phase crosslinking.
Almeida et al. [69] prepared a magnetic composite containing gra­
phene oxide, chitosan, and organoclay to remove different organic 4.1. Adsorption of heavy metals in biopolymeric adsorbents
pollutants by the crosslinking technique employing GLU at a concen­
tration of 5 % and NaOH solution for adjusting the pH. On the other Considering several side effects of heavy metals on human health,
hand, Zhang et al. [108] obtained 3D-ordered macroporous imprinted numerous searches have been developed to remove these compounds
[79,87,108,110]. Among heavy metals, lead, chromium, and copper are

Fig. 2. Effect of pH on protonation and solubilization of chitosan polymer chains.

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the most reported (Table S2). However, these results are unrelated to the 4.2. Adsorption of organic dyes using chitosan-based adsorbents
higher adsorption capacity values of chitosan-based adsorbents. Chito­
san exhibits an excellent ability to form chelates with heavy metal ions. Organic dyes are used worldwide by the food, agrochemical, phar­
This capacity results from electron-rich functional groups (hydroxyl and maceutical, and textile industries [41]. As shown in Table S3, the studies
amine). Among them, NH2 groups are more likely to form complexes are quite heterogeneous and contemplate the removal of different
with metals due to the lower ionization energy of nitrogen about the organic dyes. Among the anionic and cationic dyes, methyl orange and
oxygen atom. Thus, amine groups act as excellent electron donors for methylene blue are the most explored. Experimental conditions can
metallic cations, which can turn chitosan into a promising material for affect adsorption in batch mode. Below, a brief discussion about the
water purification [87,111]. influence of adsorption parameters on removing organic dyes in
The chelation phenomenon was also observed in a study of Cd2+ chitosan-based adsorbents was performed.
removal using Ti–Fe chitosan LDH as the adsorbent. Unlike organic Recently, Raeiszadeh et al. [32] reported methyl orange (MO)
pollutants, the adsorption of heavy metals is affected by the solution’s adsorbing using chitosan and nanodiamond-filled chitosan. The pH
pH due to metal oxides’ formation. Therefore, a narrow pH range is used study revealed that the maximum adsorption capacity for both com­
for the adsorption of these contaminants [112]. Also, the adsorption of pounds was reached at pH 4.0. Likewise, Mohamed et al. [116] found
heavy metals may be affected due to the repulsive effect between pro­ that MO adsorption employing chitosan-impregnated H2O2-activated
tonated amine groups (NH+ 3 ) and metallic ions in the acid solution anthracite as the adsorbent performed better at pH 3.0.
[6,113]. The gradual increase in the pH of the solution increases the in­
In concordance with previously reported, the pH of the solution teractions between dye-dye and adsorbent-adsorbent, resulting in
affected the removal of hexavalent chromium in the chitosan modified agglomeration and decreased adsorption efficiency [120]. Methyl or­
with vanadium pentoxide and metal-organic frameworks (MOFs). ange dye has an ionization constant (pKa = 3.46). Due to the anionic
Although the acid conditions favor the protonation of amine groups, the character, HSO3‾ groups can easily interact with the protonated amine
employ of the potassium dichromate as the chromium source (HCrO4‾) (NH+ 3 ) present in chitosan molecules and, thus, favor the adsorption
furnishes an anionic species of the heavy metal, which is easily attracted process.
by positively charged chitosan [14]. Regarding cationic dyes, the highest capacity was achieved for
The chemical composition of the adsorbent is associated with the methylene blue (2970 mg g− 1) using spherical hydrogel capsules [15].
adsorption efficiency. Diverse chitosan-based adsorbents were synthe­ The pH of the solution has a slight effect on the adsorption efficiency.
sized to remove heavy metals, such as Cr6+ adsorption [72,79,114,115]. However, the capacity values remain high, which supports a phys­
Recently, a novel adsorbent was synthesized to remove Cr6+ ions from isorption process.
aqueous solutions. The magnetic ZIF-67 MOF@aminated chitosan The high concentration of H+ ions in an acidic medium hinders in­
composite beads presented high adsorption capacity (119.05 mg g− 1) teractions between the adsorbent’s functional groups and the adsor­
and recyclability (adsorption efficiency higher than 60 %) [114]. The bate’s difficulty. Thus, Verma et al. [121] reported that the adsorption of
study by Periyasamy and Viswanathan [77], using the chitosan func­ methylene blue improved with the increase in pH. Therefore, the ideal
tionalized with hydrocalumite as the adsorbent, showed an adsorption condition for the adsorption of MB in extruded blends of activated
capacity value of 35.08 mg g− 1 at pH 3.0. Meanwhile, the H2O2-acti­ lignin-chitosan at neutral pH was observed [122]. With the gradual in­
vated anthracite impregnated with chitosan displayed a better qmax at crease in pH, it was found that the adsorbent acquires an anionic char­
pH 2.0 (201.77 mg g− 1) [116]. acter, decreasing the adsorption percentages (repulsive force between
The malic acid-enhanced chitosan hydrogel beads developed by adsorbent/adsorbent).
Zhang et al. [117], a magnetic nanocomposite produced by Reis et al. The affinity for a determined type or chemical class of adsorbate has
[79], exhibited similar behavior (adsorption capacity values were been reported in the literature [14]. Multicomponent adsorption sys­
383.15 mg g− 1 and 301.20 mg g− 1, respectively). tems have been widely explored, considering the high demand for ver­
Adsorption is a surface phenomenon; that is, the efficiency of the satile adsorbents that can simultaneously remove contaminants [15].
process is related to the specific surface area and the size of the particles Notwithstanding the adsorbents are designed with specific charac­
[118]. The adsorption intensity depends on the mass transfer resistance. teristics, the affinity of the adsorbate depends on diverse conditions. The
Thus, the diffusion of the adsorbate molecules is hampered when the adsorption can occur due to functional groups, specific surface area,
adsorbent has a high particle size, which will decrease the adsorption pore volume, pore size, and adsorbent surface charge or depending on
efficiency. However, a high specific surface area does not imply high different experimental conditions [25,104]. Furthermore, the unique
adsorption capacity values [77]. The adsorption phenomenon is not chemical structure of adsorbate may be involved in strong chemical
necessarily associated with the pore size [41,79] but is related to the interactions with the adsorbent, which confer specificity/selectivity by
affinity of functional groups on the surface [119]. adsorbate [123].
The porous carboxymethyl chitosan beads presented high-speed ki­ A binary adsorption system was developed by Zhao et al. [89]. The
netics for removing cobalt from an aqueous solution (~6 h) at an initial adsorbent exhibited a higher specificity by the Congo red than methyl
adsorbate concentration (200 mg L− 1). Nevertheless, a correlation be­ orange (the maximum adsorption capacity for CR and MO were 314.97
tween the surface area, pore size, and adsorption capacity can be and 63.23 mg g− 1, respectively).
observed. The material exhibits a low SBET value (9.36 m2 g− 1) and pore The authors did not speculate on the higher affinity for Congo red.
size of (12.81 nm), which results in a low value of qmax of 46.25 mg g− 1 However, the particularity of the chemical structure of CG (several ar­
[82]. omatic rings) and the presence of carbon nanotubes (high electron
As previously mentioned, an adsorbent with a small pore diameter density) in the composition of the nanocomposite may involve the
generally has excellent adsorption efficiency. However, the adsorbent stacking of π-π bonds [124].
had a small pore size (1.489 nm), which generally facilitates diffusion. In addition, the chitosan presents a polymer chain rich in amine
The chromium removal in the chitosan-sericin composite did not result groups, which favor the occurrence of the Yoshida H-bonding (NH2) of
in high adsorption capacity values in the study developed by Reis et al. chitosan interacting with aromatic rings of dye molecule [9]. Similar
[79]. However, the adsorption showed rapid kinetics (reached equilib­ results were reported by Eltaweil et al. [25]; the higher adsorption ca­
rium around 60 min). pacity of Cong Red about crystal violet can be attributed to the chemical
structure and explained by the possibility of different chemical in­
teractions between adsorbent and adsorbate.
Corroborating these data, chitosan spheres cross-linked with

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F. da Silva Bruckmann et al. International Journal of Biological Macromolecules 309 (2025) 143173

hexametaphosphate, used as adsorbent for Malachite green and reactive explained by the dissociation constant (pKa1 = 5.19 and pKa2 = 7.07)
red 195, showed superior performance for the anionic dye about the and surface charge of the adsorbent [127]. The solution pH also affected
cationic compound. However, several studies report the adsorption the adsorption of ciprofloxacin (CIP) into ethylenediaminetetraacetic
mechanisms between adsorbents and organic dyes involving electro­ acid-functionalized β-cyclodextrin-chitosan. The ciprofloxacin exhibits
static interactions. The present study demonstrates that the adsorption cationic characteristics with pH below 6.1 (pKa1), a neutral and slightly
of dyes may have occurred through the pores present in the adsorbent negative surface between 6.1 and 8.7, and an anionic character above
[104]. pH 8.7 (pKa2) [71].
The physicochemical characteristics of drugs: hydrophobicity,
4.3. Pharmaceutical compounds removal onto chitosan-based adsorbents chemical structure, and molecular weight can affect the interaction with
the adsorbent surface. The chemical conformation of adsorbate can
As previously reported in the literature, antibiotics are excreted in hinder the interaction with the adsorption sites due to the steric effects
high unchanged fractions (70–80 %) due to partial metabolism by [35,84,128,129]. The relation between the adsorption capacity and
human and animal organisms [125]. Therefore, this pharmaceutical better interaction with the adsorbent surface was described by Vakili
class has been widely found in wastewater and soil systems [14]. Ac­ et al. [35]. An oxidated-chitosan adsorbent was employed for penicillin
cording to shown in Table S4, it was possible to verify that only one G adsorption from aqueous solutions. The material exhibited an amor­
study showed the removal of a drug that did not involve antibiotic phous surface and shorter polymer chains, associated with higher easy
removal. This paper exhibits the adsorption of salicylic acid into mag­ adsorbate binding with the adsorbent’s functional groups. Disordered
netic chitosan nanoparticles [84]. Among these, the highest adsorption regions form amorphous materials without organized repetition of the
capacity (2165 mg g− 1) was observed for penicillin G using the oxidized atoms and molecules that form their structure. The amorphization
product of chitosan obtained mechanical technique (ball milling) [35]. procedures produce high porosity and surface area materials and syn­
As with other micropollutants, drug adsorption is also controlled by thesize an adsorbent with numerous active sites [35,130].
physicochemical properties intrinsic to the adsorbate and the adsorbent.
The pH exerts an essential tool in drug removal considering their ioni­ 4.4. Adsorption of emerging pollutants (miscellaneous) using chitosan-
zation capacity at determined experimental conditions (acid, neutral, or based adsorbents
alkaline medium) [126]. Thus, chemical species can affect adsorption
efficiency, causing an electrostatic repulsion with the adsorbent mate­ Tannic acid (TA) and humic acid (HA), key components of dissolved
rial. The influence of pH on the chemical speciation of different anti­ organic matter (DOM), are commonly found in soils and wastewater.
biotics reported in this study is shown in Fig. 3. These macromolecules can influence the removal of organic pollutants
The tetracycline (TC) is a chemical compound known for presenting by competing for adsorption sites or enhancing pollutant binding [131].
three dissociation constants (pKa1 = 3.3, pKa2 = 7.68, and pKa3 = 9.68) The binary adsorption system for removing humic acid and salicylic acid
[3,109]. The effect of pH on the adsorption behavior of TC on nitrilo­ (SA) was performed by Wang et al. [84]. The single and bi-component
triacetic acid-modified magnetic chitosan microspheres was investi­ systems were carried out to investigate the influence of the presence
gated by Tang et al. [3]. The experimental results showed that increasing of DOM. The experimental results showed that HA caused a decrease in
the pH of the solution improved the adsorption capacity values, and the the removal percentage of the salicylic acid due to high interaction with
maximum adsorption was observed at pH ~ 8.0. Based on the data, the the adsorption surface sites compared to SA. However, the adsorbent
adsorption of TC into calcined chitosan-supported layered double hy­ presents a higher specificity for SA (higher removal percentage values)
droxide was favored at the essential medium (the qmax value was than DOM. This behavior may be supported by the complexity of the
reached at pH ~ 9.0 [14]. chemical structure of humic acid, which hinders the binding with
On the other hand, the maximum removal of levofloxacin using va­ adsorptive sites.
nadium pentoxide-chitosan-MOFs occurs at pH 3.0 [12]. The results are The removal of tannic acid in chitosan composites was investigated

Fig. 3. Ionizable groups of antibiotics at different pH.

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F. da Silva Bruckmann et al. International Journal of Biological Macromolecules 309 (2025) 143173

by Agarwal et al. [20]. The influence of chitosan loading on nano­ methylparaben (MP) and propylparaben (PP) from real aqueous solution
composites was evaluated, and it was observed that an increase in the employing a magnetic compound of chitosan and activated charcoal.
percentage of biopolymer improved the adsorption efficiency. Also, the The experimental results showed that the material presents an excellent
comparative study with compounds used to synthesize nano adsorbent performance for the removal of these preservatives, but adsorption ca­
revealed that the adsorption of TA was enhanced with the chitosan- pacity values were similar (MP (85.9 mg g− 1) and PP (90.0 mg g− 1)).
nanocomposite. The phosphate ions are sorted as the aquatic contaminant. The
The adsorption mechanisms are related to the chemical structure of presence of these PO3‾4 anions is commonly from human activity through
DOMs. The removal of humic acid occurred mainly by the hydrophobic the fertilizer and pharmaceutical industries, sewage (soap and deter­
interactions (π-π), H-bonds, and charge transfer. Meanwhile, the in­ gent), and naturally occurring (rocks). At determined concentrations
teractions reported for the adsorption of tannic acid in chitosan nano­ can cause the eutrophication process and aquatic toxicity [136,137].
composite and fly ash was a chemisorption phenomenon by hydrogen Eltaweil et al. [138] prepared a more selective adsorbent for anions
bonds. by synthesizing Lanthanum-based materials. The adsorbent with higher
Organic compounds assemble substances among these, including Lanthanum content exhibited the highest removal efficiency and
polycyclic aromatic hydrocarbons (PAHs) and phenolic compounds. adsorption capacity.
These compounds, such as bisphenols, are classified as emerging and At the same time, fluoride ions are ubiquitous in the groundwater
hazardous pollutants due to numerous side effects on humans and ani­ and widely employed in the pharmaceutical industry. Although it is an
mals [95]. Anthropogenic activity, mainly related to industrial processes essential element for health, high concentrations are involved with side
and petroleum refining, are common sources of PAHs. effects on the body, such as cognitive deficit, cytotoxicity, and thyroid
Regarding bisphenol A, this compound is widely used by the plastics disorders, among others [139]. Similarly, contamination by sulfate ions
industry and is present in several household products. Therefore, its is currently due to mining activity, acid leaching, and rock weathering
presence in animals, blood, groundwater, and soils has been docu­ [140]. The water persistence and high concentrations can affect the
mented [132]. At the same time, ethinylestradiol (EE2) is also known for salinity of fresh waters, altering the aspect and flavor [141].
its notorious effects on humans and fish [133]. Recent reports have documented the remediation of these ions by
Herein, the main aspects of the remediation of these compounds employing the adsorption process. Kumar et al. [139] reported a study of
were reported in the [95] and Patiño-Ruiz et al. [74]. Both studies were fluoride adsorption from aqueous solutions using different ferrites.
performed with composites containing chitosan, titanium, and iron Among these, chitosan-modified nickel ferrite showed slightly higher
particles but synthesized by different techniques. adsorption capacity and removal percentage values than other magnetic
The study removal of naphthalene into chitosan-thiourea-Fe3O4- chitosan composites (cobalt and zinc ferrites). The adsorption was
TiO2 and chitosan-thiourea revealed an insignificant effect of chitosan affected by the surface area of the adsorbent, although a slight difference
modification with magnetite and titanium oxide nanoparticles. For between the materials was observed.
instance, the maximum adsorption capacity values were 133.69 and Newly, a ferrocene-functionalized chitosan aerogel (Fc-Cs) [142]
133.652 mg g− 1, respectively. The main reason explained by the authors and Ti–Fe chitosan LDH [112] were employed in an adsorption system
is the type of interaction between NH+ 3 groups (chitosan) and aromatic for the removal of phosphate ions. A comparative analysis between
rings (naphthalene). communications showed that phosphate removal is not associated with
Concerning the reports of Patiño-Ruiz et al. [74], the adsorption of available adsorption surfaces. The double hydroxide adsorbent had a
naphthalene in chitosan modified with FeO and TiO2 nanoparticles (Ch- high specific area (146 m2 g− 1) and lowest adsorption capacity (40.00
FeO/TiO2) and unchanged chitosan (un-Ch) occurred a distinct manner. mg g− 1). On the other hand, the ferrocene-chitosan composite exhibited
While the adsorption capacity of un-Ch was 70.9 mg g− 1, the maximum a low surface area (5 m2 g− 1) and resulted in an excellent adsorption
value for Ch-FeO/TiO2 was 149.3 mg g− 1. These results are supported by capacity (1141 mg g− 1).
the effect of titanium and magnetite nanoparticles that improved the The adsorption of phosphate ions using Ti–Fe chitosan LDH was
surface adsorption area of the adsorbent. Although the materials pre­ performed in multicomponent adsorption with a heavy metal (Cd2+) and
sented different values for the specific surface area (for example, Ch-T- benzoquinone. The competitive assay revealed that the adsorbent had a
M-Ti presented an SBET of 1.582 m2 g− 1, while Ch-FeO/TiO2 presented a higher affinity for benzoquinone than for cadmium and the inorganic
value of 27.1 m2 g− 1), the values for the adsorption capacity were element, as it showed less variation in the adsorption capacity in the pH
similar, which demonstrates that the textural property had no influence range studied.
on the adsorption process but was influenced by the chemical compo­ Along with this, the adsorption of sulfate ions was investigated using
sition of the adsorbent. biopolymer-based ternary metal composites (containing chloride, ni­
Likewise, a comparative study was also carried out between chitosan trate, and sulfate). Among, adsorbents containing chloride showed a
and chitosan-grafted multiwall carbon nanotubes (MWCNTs) for phenol better performance due to the higher availability of adsorption sites
removal. The results showed that the nanocomposite exhibited higher [10]. The water contamination by rare earth and selenium also repre­
adsorption capacity than pure biopolymer [21]. sents an environmental problem. Selenium (Se) is a metalloid belonging
Similarly, the removal of other toxic organic contaminants was also to a group of chalcogens with diverse beneficial effects on the body.
investigated. Almeida et al. [69] explored the adsorption of three However, this element has been associated with diverse side effects at
emerging pollutants: bisphenol A, ethinylestradiol, and triclosan, using higher concentrations, such as neurodegenerative diseases and carci­
a composite of graphene oxide, magnetic chitosan, and organoclay (GO/ nogenesis [143]. The contamination of water by Se occurs in several
mCh/OC) and pure organoclay. This study revealed that both adsorbents ways, either by natural origin or from human activity.
performed better adsorbing the triclosan (higher adsorption capacity Considering these compounds’ water contamination and bio­
and removal percentage values) than other adsorbates. Nevertheless, the accumulation, remediation studies have been developed using the ter­
magnetic nanocomposite and pure organoclay exhibited similar tiary method (adsorption) (Table S5). The removal of selenium species
behavior in triclosan removal. was investigated by Li et al. [144] and Song et al. [66] using a chitosan-
Although preservatives are indispensable in manufacturing personal adsorbent containing layered double hydroxide and sludge-based bio­
care products, drugs, and other materials, paraben is a class of com­ char/chitosan, respectively. Li et al. [144] study showed that the
pounds commonly employed in developing cosmetics products due to its adsorption of selenium species (Se4+ and Se6+) occurred by different
excellent antimicrobial activity [134]. However, studies have associated mechanisms involving chemical interactions and ion exchange, respec­
exposure to compounds with endocrine dysfunction [135]. tively. When comparing the adsorption efficiency, the adsorbent showed
Recently, relevant research reported the simultaneous removal of similar values for the adsorption capacity (Se4+ (17 mg g− 1) and Se6+

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F. da Silva Bruckmann et al. International Journal of Biological Macromolecules 309 (2025) 143173

(~12 mg g− 1)). interaction between adsorbate and adsorbent. However, in some con­
However, the sludge-based biochar/chitosan exhibits a lower ditions, weak interactions (Van der Waals) in the adsorbent surface with
adsorption capacity (0.034 mg g− 1) than the LDH-chitosan nano­ the dosage increase decreases surface area and adsorption efficiency
composite. This result can relate to the initial concentration of adsorbate [109].
(0.008 mg L− 1) and adsorbent dosage (0.5 g L− 1) employed in the Recently, Figueiredo Neves et al. [24] reported that the increase in
adsorption assay. Regarding removing REMs, a magnetic bio-adsorbent adsorbent concentration improved the removal values but caused a
was used in the study. The maximum adsorption was reached at pH = decrease in adsorption capacity due to an unbalance between the ratio
7.0 at room temperature. In addition, the kinetic and isotherms adsorbate: adsorbent. Guo et al. [21] concluded that the adsorption of
modeling suggests the dual behavior, i.e., different adsorption mecha­ phenol onto carbon nanotubes-grafted chitosan was enhanced initially
nisms can occur depending on adsorbate concentration. with the adsorbent dosage. However, after a specific concentration, the
number of adsorbed phenol molecules decreased due to unoccupied
5. Effect of experimental conditions on the adsorption process adsorption sites (many adsorbent sites for a few adsorbate molecules).

5.1. Effect of pH 5.3. Effect of temperature

The experimental procedure to verify the adsorbent’s surface charge Temperature is an essential experimental parameter that is involved
provides the material’s character as a function of pH. The effect of pH in with adsorption efficiency. Thus, the temperature can further increase
the diverse microcontaminant adsorption process has been widely re­ the adsorption capacity due to improving molecule diffusion through
ported. Elwakeel et al. [7] related that the maximum adsorption ca­ the boundary layer overcoming the mass transfer resistance. The
pacity of MB in the 2-MBI-Chitosan was reached at alkaline pH (9.3). adsorption capacity of MB in porous chitosan derivatives increased
The double effect on the degree of chemical compound speciation around 50 mg g− 1 when the temperature changed from 298 to 318 K [4].
(adsorbent and adsorbate) was observed in this study. The pH caused the Similarly, the adsorption of phenol onto carbon nanotube-grafted chi­
ionization of molecules in the solution, hampering the sorption process. tosan was also improved with the temperature. Furthermore, the nega­
Sadiq et al. [88] investigated the adsorption of cationic dye (MG) in tive values of Gibbs free energy (ΔG) showed the affinity of the
chitosan-based nanocomposites. The nano adsorbents presented pHZCP adsorbent for the adsorbate, which favors the adsorption process [21].
~ 6.5, i.e., compounds presented a surface of positive charge when pH Meanwhile, the temperature influence study reported by Agarwal
< pHZCP, favoring the interaction with the cationic dye. The optimal et al. [20] describes that tannic acid removal was negatively affected by
condition for green malachite removal was achieved at acidic pH, and increasing temperature, typical of an exothermic process. At the same
the electrostatic interaction controls the adsorption process. time, the adsorption of levofloxacin was also impaired by the increase in
Raeiszadeh et al. [32] reported that the adsorption of methyl orange temperature [14].
(anionic dye) on chitosan/nanodiamond nanocomposites occurred more The deactivation of active sites and pore destruction can support a
significantly in the acid medium (pH 4.0) As the functional groups of the decrease in the adsorption values. Further, exothermic processes
adsorbent are easily protonated under acid conditions, attractive forces generally involve the physisorption phenomena that are affected by the
between molecules are favored. temperature (weak interactions) [109,145]. On the other hand, tem­
The structural complexity (presence of diverse organic functions) perature can also improve the process due to increased surface area,
allows the ionization of functional groups and the formation of chemical pore size, and collision between particles [139].
species. Newly, [3] developed a magnetic chitosan nanocomposite for
tetracycline removal from aqueous solutions. Thus, it was observed that 5.4. Effect of ionic strength
the pH affects the adsorption process, suggesting that the adsorption
capacity is improved with the increase of pH of the solution (pH 8–9). Coexisting ions and ionic strength are important conditions to be
The pH also plays an important role in heavy metals removal. Zhang explored as they are commonly found in wastewater [41]. The ions can
et al. [117] report that chromium and copper adsorption was signifi­ affect the adsorption in two manners: improving the adsorption capacity
cantly affected by the pH of the solution. H+ and ‾OH ions in an by increasing the aqueous solubility of adsorbate molecules and the
adsorption system can interfere with the complexation mechanisms and surface area of the adsorbent or reducing the adsorption performance
cause metal precipitation. through the competition by the adsorption sites [146,147].
Singh et al. [41] evaluated the influence of different inorganic salts
5.2. Influence of initial concentration of adsorbate and adsorbent dosage and ionic strength on the adsorption behavior of MO. They observed that
the adsorbent exhibited high specificity for the pollutant, the adsorption
Higher initial pollutant concentrations commonly enhance mass not affected by the coexisting ions and only by sodium chloride in so­
transfer to the solid surface by increasing the concentration gradient and lution. As aforementioned, the removal of MO into nanodiamond-filled
promoting competition for adsorption sites [3,95]. Hui et al. [16] chitosan is also hampered by the ionic strength (KCl and NaCl) [32]. On
showed that the Congo red adsorption onto magnetic chitosan fluid the other hand, Sadiq et al. [88] reported that the decrease in malachite
(MCF) depends on initial CR concentration. The gradual increase of the green adsorption resulted from the increase in pH caused by the salt,
CR concentration resulted consequently an increase in the adsorption which affects the interactions between the adsorbent and adsorbate. The
capacity. Although the adsorbent adsorption capacity increased with the interactions between TC and nitrilotriacetic acid-modified magnetic
adsorbate concentration, a reduction in the removal percentage was chitosan were also interfered with by the NaCl solutions; the adsorbent
observed, possibly due to the saturation of the binding sites. content (nitrilotriacetic acid) has the capacity for chelation reactions
Corroborating this result, the percentage of ferric ion removal with cations, which hampering its binding with the drug [3].
decreased with a gradual increase in the adsorbate concentration [113]. Elwakeel et al. [148] also reported the shielding effect by investi­
Likewise, the heavy metals and organic dye removal study developed by gating the influence of ionic strength on methylene blue adsorption.
Verma et al. [121] demonstrated that increasing the initial adsorbate However, despite NaCl affecting the process, the removal percentage
improved the adsorption capacity values but caused a reduction in the decreased by around 24 % using a high salt concentration (0.77 mmol
removal percentages. L− 1).
Meanwhile, the adsorbent dosage can improve the adsorption ca­
pacity and removal percentage. The rise of adsorbent mass enables a
higher specific surface area and adsorption sites, which allows the best

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F. da Silva Bruckmann et al. International Journal of Biological Macromolecules 309 (2025) 143173

5.5. Effect of loading percentage on the composite material 7. Future perspectives on chitosan-based adsorbents

Another parameter that may be involved with the adsorption per­ Although chitosan-based adsorbents have demonstrated remarkable
formance is the adsorbent constituents. Agarwal et al. [20] synthesized a performance at the laboratory scale, their application under real oper­
nanocomposite containing diverse chitosan content (2.5–10.0 wt%). ational conditions still faces significant challenges. In addition to limi­
Initially, the biopolymer charge improves the adsorption capacity tations related to practical usage conditions, the production of chitosan
values. However, at a high percentage, the process was impaired due to itself can be complex, often requiring multiple chemical reagents and
the agglomeration of CS that prevented the interaction of the adsorbate several processing steps. These factors may compromise the reproduc­
molecules. ibility of the material and considerably increase production costs.
Shehap et al. [113] recently documented the efficiency of chitosan- Despite these difficulties, chitosan is one of the most promising bio­
nanocomposites containing different percentages of chitosan/montmo­ polymers for environmental applications due to its renewable origin,
rillonite (CS/MMT) for an adsorption study of Fe3+. The results showed high chemical reactivity, strong adsorption potential, and environmen­
that composites with chitosan contents above 50 % resulted in brittle tally friendly profile.
films. Among the synthesized adsorbents, the adsorbent containing Adopting continuous and standardized production methods is a
(40–60 wt%) of CS/MMT showed the highest adsorption performance promising strategy to enable the large-scale use of chitosan. Flow-
(89.2 %). Effects on the specific surface area are the reason for a through processes and desorption studies have gained increasing
decrease in the maximum adsorption capacity of methyl orange using attention in the scientific literature, including the works reviewed in this
chitosan nano adsorbent with different contents of nanodiamond (%). paper. These approaches offer greater control over synthesis parameters,
The gradual increase in the quantity of carbon nanoparticles results in an improve reproducibility and reusability, and facilitate material scal­
agglomeration in the polymer matrix, reducing the surface area [32]. ability. As a result, they contribute significantly to making the produc­
tion of modified chitosan more efficient, economically viable, and
6. Desorption and regeneration compatible with industrial demands—thereby expanding its potential
for use in water treatment under realistic conditions. Moreover, the
The desorption studies are crucial steps considering the ecologically possibility of structural modifications, polymer blending, and magnetic
correct approach, the costs involved with the process, evaluating the functionalization of chitosan-based adsorbents has opened new avenues
performance of the adsorbent under various adsorption-desorption cy­ for their recovery and reuse in treatment systems.
cles, the best eluent, as well as determining the useful life of the material Therefore, to move toward practical applications, future research
[72,148,149]. should prioritize the development of simplified and cost-effective
Table S6 summarizes the different eluents used in the desorption modification methods aligned with green chemistry principles, aiming
studies for chitosan-based adsorbents as wand efficiency after diverse to address complex pollution scenarios with high efficiency and minimal
sorption cycles. As observed, most reports documented the regeneration environmental impact.
of adsorbents using NaOH and HCl. Among them, hydrochloric acid was
the most used as a desorbing agent for organic dyes in its pure form or 8. Conclusions
combined with ethanol, while sodium hydroxide was the most used for
the desorption of heavy metals. The comprehensive review reported the synthesis and application of
In addition, the materials perform well in the adsorption process, chitosan-based adsorbents as the strategy for water remediation using
maintaining efficiency after successive adsorption/desorption cycles. the adsorption process. This study allowed an approach to the effect of
Moreover, adsorbents with magnetic behavior have advantages over chemical modification on the characteristics and properties of adsor­
non-magnetic materials, as they can be easily separated from aqueous bents. Crosslinking reactions were the most used to modify the structure
solutions by applying an external magnetic field, avoiding the steps of of chitosan, using the glutaraldehyde crosslinker agent. Meantime, co-
filtration and centrifugation. precipitation was the methodology most used for obtaining the
The material’s desorption efficiency and adsorption capacity are magnetite-functionalized chitosan. However, chemically modified chi­
related to the regeneration capacity (incomplete desorption) and the tosan indicated limited availability due to the experimental process
type of interaction. The regeneration study of mCHBs saturated with needed for production, which hindered large-scale applications.
Cu2+ was developed using EDTA at different concentrations. After six The characterization techniques showed that the modifications in the
cycles, it was possible to verify a slight decrease in the qmax, which can polymer structure improve the thermal and physicochemical stabilities
be attributed to the chemical interaction between adsorbent/adsorbate as well as facilitate the recovery of the adsorbent from the aqueous
[117]. Similarly, Figueiredo Neves et al. [24] reported low desorption medium due to the magnetic behavior by the simple approximation of a
efficiency, suggesting strong interactions between mCS/GO-QAS and simple magnet avoiding the filtration and centrifugation steps.
BB4. In addition, including other compounds changed crystalline,
The type of interaction also affected the desorption efficiency of textural, and morphological characteristics. The adsorbents generally
MNCDES and PCCDES saturated with MG. Weak interaction (phys­ exhibited a higher surface area than pure chitosan.
isorption phenomenon) resulted in high desorption percentages [88]. In Regarding adsorption studies, most reports documented the removal
addition, a reduction in the adsorption efficiency may be related to of heavy metals and organic dyes. Methylene blue (2970 mg g− 1) re­
incomplete desorption (inadequate eluent), chemical modifications in ported a high adsorption capacity using spherical hydrogel capsules.
the adsorbent structure, and mass losses during the adsorbent recovery Adsorption is a complex process because it involves several experi­
[16,35]. mental parameters and characteristics intrinsic to the adsorbent. Thus,
Chemically modified chitosan poses significant limitations for large- adsorption efficiency involves temperature, ionic strength, pH, adsor­
scale applications due to its non-abundant availability. Acquiring this bent dosage, and adsorbate concentration. Also, different mechanisms
modified material requires intricate experimental preparation involving are related to the adsorption of emerging pollutants, such as hydrogen
multiple chemical steps to achieve optimal results. Beyond its scarcity, bonds, organic partition, electrostatic interactions, ion exchange, che­
the complex experimental process also contributes to the difficulty of lation, and hydrophobic interactions, among others, depending on pH,
large-scale production. The need for several additional chemical steps the chemical structure of adsorbent, and adsorbate. In summary,
raises the costs associated with production and adds logistical chitosan-based materials showed excellent performance in the adsorp­
complexity to the process. Therefore, considerations regarding eco­ tion of pollutants emerging from real aqueous solutions, overcoming the
nomic feasibility and scalability are essential. limitations of the pure biopolymer.

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F. da Silva Bruckmann et al. International Journal of Biological Macromolecules 309 (2025) 143173

CRediT authorship contribution statement [11] Y. Liu, Y. Gao, B. Yao, D. Zou, Removal of chlortetracycline by nano- micro-
electrolysis materials: application and mechanism, Chemosphere 238 (2020)
124543, https://doi.org/10.1016/j.chemosphere.2019.124543.
Franciele da Silva Bruckmann: Writing – review & editing, Su­ [12] S. Suarez, J.M. Lema, F. Omil, Pre-treatment of hospital wastewater by
pervision, Project administration, Funding acquisition, Conceptualiza­ coagulation–flocculation and flotation, Bioresour. Technol. 100 (2009)
tion. Janaína Oliveira Gonçalves: Software, Resources, Methodology, 2138–2146, https://doi.org/10.1016/j.biortech.2008.11.015.
[13] X. Li, Z. Zhang, A. Fakhri, V.K. Gupta, S. Agarwal, Adsorption and photocatalysis
Investigation, Formal analysis, Data curation. Luis Felipe Oliveira assisted optimization for drug removal by chitosan-glyoxal/
Silva: Validation, Supervision, Project administration, Funding acqui­ Polyvinylpyrrolidone/MoS2 nanocomposites, Int. J. Biol. Macromol. 136 (2019)
sition. Marcos Leandro Silva Oliveira: Visualization, Validation, 469–475, https://doi.org/10.1016/j.ijbiomac.2019.06.003.
[14] M.E. Mahmoud, M.F. Amira, M.M.H.M. Azab, A.M. Abdelfattah, Effective
Software, Resources, Methodology, Investigation, Formal analysis. removal of levofloxacin drug and Cr(VI) from water by a composed
Guilherme Luiz Dotto: Writing – review & editing, Writing – original nanobiosorbent of vanadium pentoxide@chitosan@MOFs, Int. J. Biol. Macromol.
draft, Supervision, Project administration, Funding acquisition, 188 (2021) 879–891, https://doi.org/10.1016/j.ijbiomac.2021.08.092.
[15] X. Huang, D. Zhou, Y. Wang, C. He, W. Zhao, S. Sun, C. Zhao, A green approach
Conceptualization. Cristiano Rodrigo Bohn Rhoden: Writing – review towards functional hydrogel particles from synthetic polymers via spherical
& editing, Writing – original draft, Visualization, Validation, Supervi­ capsule mini-reactors, Chem. Eng. J. 359 (2019) 1360–1371, https://doi.org/
sion, Conceptualization. 10.1016/j.cej.2018.11.042.
[16] M. Hui, P. Shengyan, H. Yaqi, Z. Rongxin, Z. Anatoly, C. Wei, A highly efficient
magnetic chitosan “fluid” adsorbent with a high capacity and fast adsorption
Declaration of competing interest kinetics for dyeing wastewater purification, Chem. Eng. J. 345 (2018) 556–565,
https://doi.org/10.1016/j.cej.2018.03.115.
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