A Comprehensive Review of Polysaccharide-Based Hydrogels as Promising Biomaterials
Abstract
:1. Introduction
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- To classify hydrogels based on various factors (source, cross-linking method, polymer composition, crystallinity, electrical charge, form, and pore size);
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- To provide an overview of the basic research on natural hydrogels based on chitosan, cellulose, starch, and other polysaccharides;
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- To summarize the various methods of hydrogel synthesis and provide information on hydrogel characterization;
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- To give a view of the various applications of polysaccharide-based superabsorbent polymers;
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- To discuss the practical applications of hydrogels based on polysaccharides in various fields, including agriculture, wastewater treatment, and biomedical engineering;
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- To identify the current technology’s challenges and limitations and suggest future research and development directions.
2. Classification of Superabsorbent Polymers
2.1. Source
2.1.1. Hydrogels Based on Natural Polymers
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- Polysaccharide-based hydrogels
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- Hydrogels based on polypeptides
2.1.2. Hydrogels Based on Synthetic Polymers
2.1.3. Hybrid Hydrogels
2.2. Type of Cross-Linking
2.3. Polymer Composition (or Network Nature)
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- Homopolymeric hydrogels: Their network is made from a single species of monomer, which serves as the network’s basic component [35]. This monomer can be cross-linked according to its nature and the polymerization process;
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- Copolymeric hydrogels: Its network comprises two or more distinct monomers, at least one of which is hydrophilic, arranged in a random configuration, sequenced or alternated along the polymeric network’s chain [36];
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- Interpenetrated polymer network (IPN) hydrogels: They consist of two independently bonded natural and/or synthetic polymers arranged as a network, where just one is cross-linked. They are synthesized by immersing a pre-polymerized hydrogel in a monomer solution in the presence of an initiator [37]. In addition, these hydrogel systems have better fracture toughness with maximum compressive stress than traditional hydrogels, owing to the ability of one network to maintain the SAP’s elasticity. Another ability is to self-heal when the charge is removed, such as for the SAP prepared from elastic chemical cross-links and self-healing physical cross-links formed together to ensure entanglement [38].
2.4. Crystallinity (Network Morphology)
2.5. Electrical Charge or Ionic Particles
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- Non-ionic;
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- Ionic (anionic or cationic);
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- Amphoteric (ampholytic) electrolyte, containing acid and basic groups;
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- Zwitterionic, containing anionic and cationic groups in each repetitive unit.
2.6. Form
2.7. Pore Size
3. SAPs Based on Polysaccharides: Synthesis and Types
3.1. Polysaccharides
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- Animal polysaccharides: Divided into glycosaminoglycans (such as hyaluronic acid, heparin, and keratan sulfate) and chitin/chitosan. They comprise many functional groups such as -NH2, -OH, -COOH, and -SO3H;
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- Plant polysaccharides: Generated from plant cell metabolites. The most abundant are starch and cellulose;
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- Microbial polysaccharides: Produced by many bacteria such as Pseudomonas elodea and Sphingomonas paucimobilis.
3.2. Methods of Preparing Natural SAPs
3.2.1. Physical Cross-Linking: Reversible Hydrogels
3.2.2. Chemical Cross-Linking: Permanent Hydrogels
3.3. Cellulose-Based Hydrogels
3.4. Chitosan-Based Hydrogels
3.5. Starch-Based Hydrogels
3.6. Composite Hydrogels
3.7. Hydrogels Based on Other Polysaccharides
4. Bio-Based SAP Characterization
4.1. Gel Fraction Study
4.2. Structural Analysis
4.2.1. FTIR
4.2.2. NMR
4.2.3. XRD
4.2.4. UV–Vis
4.2.5. Raman
4.3. Morphological Analyses
4.3.1. SEM
4.3.2. AFM
4.4. Mechanical and Thermal Analyses
4.4.1. Thermal Analysis
4.4.2. Mechanical Analysis
Dynamic Mechanical Analysis
Rheology
4.5. Biodegradability
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- Soil burial: An established and standardized technique where the tested SAP is buried in soil, then washed and weighed after a defined time, and the result is expressed as a weight loss percentage for a predetermined time [213].
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- Microbial degradation: Using a microbial oxidative degradation analyzer, the hydrogel is mixed with sea sand and compost, calculating the quantity of dissipated CO2 and producing H2O during degradation [217].
4.6. Swelling Mechanism of Hydrogels in Water and Various Parameters Affecting It
4.6.1. Reagents’ Concentration Effect
Effect of Initiator Concentration
Effect of Cross-Linker Concentration
Effect of Monomer Ratio
4.6.2. Temperature Effect
4.6.3. pH Effect
4.6.4. Ionic Strength Effect
4.7. Loading and Release of Nutrients
5. Applications of Polysaccharide-Based Superabsorbent Polymers
5.1. Agriculture
5.1.1. Water Reservoir
5.1.2. Slow/Controlled-Release Fertilizers
5.2. Wastewater Treatment
5.3. Biomedicine
5.4. Other Applications
6. Conclusions
7. Prospects
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- The hydrogel field has received great attention from researchers to improve their environmental responses to promote their application in various fields. Indeed, the focus should be on natural hydrogels, biohydrogels, which are biodegradable, non-toxic, economical, and more sustainable, especially in medical fields, agriculture, food industries, and water purification systems, so as not to affect the environment and human health, while avoiding an increase in the current plastic soup caused by hydrogels based on petrochemical polymers, having a huge environmental impact.
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- This type of superabsorbent polymer has many more beneficial properties than synthetic SAPs, given the economic and environmental side. However, there are still some challenges to overcome, such as limiting the formulation complexity of some SAPs, such as chitosan-based hydrogels, as it is known that chitosan is difficult to dissolve without using acids for a long time.
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- The importance of extracting polysaccharides from some wastes to make hydrogels instead of commercialized ones should be recognized to reduce the product’s cost and valorize industrial wastes. In addition, incorporating waste materials into hydrogels as reinforcements can be a solution to valorize some waste materials and also improve the mechanical and adsorption/absorption properties.
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- It is necessary to agree on a general protocol to be followed or to set a uniform standard for the calculation of the absorption and water retention capacity of hydrogels while defining standard conditions to be applied, such as the duration of the test, temperature, and humidity, to compare the results of one hydrogel with others.
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- In the agricultural field, it is necessary to try to include swelling tests in the soil because the SAP’s ability for absorption in the soil is not as good as in laboratory-scale absorption experiments since some conditions are not controllable, such as temperature, humidity, and pH of the irrigation water.
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- As synthetic hydrogels are still applied in several sectors, semi-synthetic hydrogels, known as intelligent SAPs, will require a lot of research efforts in the future, as this combination of natural and synthetic polymers will improve the durability of these synthetic hydrogels.
Author Contributions
Funding
Institutional Review Board Statement
Data Availability Statement
Acknowledgments
Conflicts of Interest
References
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Physical Cross-Linking | Chemical Cross-Linking | |
---|---|---|
Advantages | - Reversible - No need for a cross-linking agent - No need to remove the solvent’s residual amount - Excellent shear recovery (self-healing hydrogels) - Simple preparation process | - Permanent - Provides high mechanical strength - Easily approachable - Highly efficient and more controllable - Provides high molecular weight |
Disadvantages | Poor mechanical strength | Need for a purification step |
Techniques | ||
Characteristics | - Formation of non-covalent electrostatic interactions - Possibility of preparation without chemical modification of the polymers | - Formation of covalent bonds - Use of cross-linking agent - Presence of some chemical reactions |
Unbranched | Branched | Reference | |
---|---|---|---|
Homopolysaccharides | [43] | ||
Heteropolysaccharides | |||
Each of these forms below represents a different monosaccharide. Hexose: Glc Man Gal HexNac: GlcNAc ManNAc GalNAc |
Polysaccharide (Subunit, Bonds) | Structure | Source | Characteristics (In Addition to Low Cost, Biodegradability, Eco-Friendliness, High Biocompatibility, Multifunctionality) | Ref. |
---|---|---|---|---|
Animal Polysaccharides | ||||
Chitin (N-acetyl glucosamine, β1–4) | Exoskeletons of fungus, mollusks, insects, and crustaceans | - Unbranched homopolysaccharide. - The most abundant animal polysaccharide on Earth. - Present in three crystalline structures: alpha, beta, and gamma. - Renewable, with high hydroxyl, amino, and acetyl group content. - Poor solubility in solvents. | [46,47] | |
Chitosan (glucosamine and N-acetyl glucosamine, β1–4) | Chitin (via deacetylation) | - Unbranched homopolysaccharide. - Crystalline, cationic, and hydrophilic. - Possesses amino and hydroxyl groups. - Low solubility in many solvents, soluble in dilute acidic solutions. - Sophisticated extraction processes. - (-NH2) groups facilitate chemical cross-linking to make SAPs. - Its derivatives are procured via graft copolymerization, thiolation, and carboxymethylation, among other modifications. - Excellent adsorption capability. - Very viscous polymer solution. | [48,49,50] | |
Hyaluronic acid (D-glucuronic acid, N-acetyl glucosamine, β1–4 and β1–3) | Extracellular matrix of soft connective tissues and skin | - Unbranched heteropolysaccharide. - Its solution is viscoelastic at higher concentrations. - Need for chemical modification or covalent cross-linking. - Makes chemical hydrogels. - Excellent water-holding capacity and viscoelastic properties. | [51] | |
Plant Polysaccharides | ||||
Cellulose (D-glucopyranose, β-1–4) | Green plants (like bamboo and trees), natural fibers, bacteria | - Unbranched homopolysaccharide. - Earth’s most abundant organic substance. - Semi-crystalline, with a high density of (-OH) groups. - -OH in positions C2, C3, and C6 can serve as reactive groups for modifications, such as esterification or etherification of -OH, to produce some derivates (such as hydroxyethyl cellulose, hydroxypropyl cellulose, and carboxymethyl cellulose) for making various types of SAPs. - Difficult dissolution in water because of its crystalline regions linked by intra- and inter-molecular H-bonds. - Dissolves in organic solvents, alkali/urea aqueous medium, and ionic liquids. | [52,53,54,55,56,57] | |
Starch (amylose (α-1,4-linked D-glucose) and amylopectin (α-1,4- and α-1,6-linked D-glucose)) | Crop seeds, potato, corn, roots, and stalks | - Branched heteropolysaccharide. - Insoluble in alcohol, cold water, or other solvents. - Composed of linear amylose (20–30%, semi-crystalline, soluble in hot water) and branched amylopectin (70–80%, highly crystalline, insoluble in hot water), with numerous hydroxyl groups. - Has a source-dependent structure. - Swells in water at ambient temperature. - Inexpensive and easy to modify with other polymers. | [58,59] | |
Pectin (D-galacturonic acid connected by 1→4 glycosidic bonds) | Cell walls of higher plants (e.g., black currants and apples) (Extraction with water) | - Unbranched heteropolysaccharide. - Anionic polysaccharide with hydroxyl, ester, and carboxyl groups. - Soluble in water. - Categorized according to the methoxy content: high-methoxy pectins (>50% esterified), which form gels at low pH, and low-methoxy pectins (<50% esterified), which form partially sheared gels. | [60] | |
Alginate (guluronic acid and mannuronic acid, β-1→4 glycosidic bonds) | Brown seaweeds (Via treatment with aqueous alkali solutions, generally NaOH) | - Unbranched heteropolysaccharide. - Anionic polysaccharide, flexible, strong, and water soluble. - Possibility of adjusting its properties by changing the guluronic acid/and mannuronic acid ratio. - Commercially available as sodium alginate. - Makes generally physical SAPs by the addition of divalent cations. | [61,62,63,64] | |
Agarose (3,6-anhydro-α-L-galactopyranosyl and β-D-galactopyranosyl) | Red algae of seaweeds, e.g., Gelidium and Gracilaria | - Unbranched heteropolysaccharide. - Insoluble in cold water but soluble in hot water, forming a gel after cooling down. - Neutral and thermo-responsive polysaccharide. - Excellent water retention capability. | [65] | |
Carrageenan (β-(1→4)-3,6-anhydro-D-galactose and α-(1→3)-D-galactose) | κ-carrageenan | Rhodophyceae red seaweeds | - Unbranched heteropolysaccharide. - Possesses many carboxyl and hydroxyl groups, with one sulfate group for kappa (κ), two sulfate groups for iota (ι), and three sulfate groups for lambda (λ) per unit. - κ-carrageenan and ι-carrageenan form stable physical hydrogels. | [66,67] |
Guar gum (1,4-linked β-D-mannopyranose and 1,6-linked α-D-galactopyranose) | Seeds of Cyamopsis tetragonolobus | - Branched heteropolysaccharide. - Non-ionic polysaccharide. - Rapidly swells and produces viscous solution even in cold water. - Contains hydroxyl groups, which can be reactive for chemical modifications, such as introducing -COOH, -NH2, and -SO3H groups. | [68,69] | |
Cyclodextrin (D-glucose, α1–4-glycosidic bonds) | Enzymatic conversion of starch | - Unbranched heteropolysaccharide. - Cyclic structure of 6, 7, or 8 units: α-cyclodextrin (6 subunits), β-cyclodextrin (7 subunits), and γ-cyclodextrin (8 subunits). - High stability against amylase. - Cyclic structure with an interior hydrophobic cavity and a hydrophilic external surface. | [70] | |
Microbial Polysaccharides | ||||
Pullulan (maltotriose, α-(1–6) and α-(1–4) glycosidic bonds) | The fungus Aureobasidium pullulans | - Unbranched heteropolysaccharide. - Has nine -OH groups per unit, with great mechanical properties. - High chemical reactivity and water soluble. - Possibility of chemical modification (etherification, esterification, sulfonation, or oxidation) for making various hydrogels. | [71,72] | |
Dextran (D-glucose, α-(1–6) with branches of α-(1–3)) | Lactic acid bacteria, e.g., Streptococcus, Leuconostoc, Weisella, and Lactobacillus | - Branched homopolysaccharide. - Non-ionic flexible structure due to free rotation of glycosidic bonds. - Water insoluble (with the existence of >43% of α-(1–3) linking branches), and water soluble (with 95% linear linkage). - Capable of being modified to form dextran sulfate and cationic dextran, for making diverse SAPs. | [73] | |
Salecan (β-1,3-glucose) | Agrobacterium sp. ZX09 | - Unbranched homopolysaccharide. - Contains hydroxyl groups, soluble in water. - Has good rheological properties and forms high-viscosity solutions at low doses and shear stresses. | [74,75] | |
Gellan gum (D-glucose, D-glucuronic acid, and L-rhamnose) | Bacteria, like Sphingomonas paucimobilis and Pseudomonas elodea | - Unbranched heteropolysaccharide. - Anionic and possesses many active groups: -OH and -COOH, with the possibility to obtain deacylated gellan gum by modification. - Forms physical SAPs while cationic ions such as Na+ and Ca2+ are present at low temperatures. | [76] | |
Xanthan gum (D-glycopyranose linked with a side chain via α-1,3 linkage) | Bacteria Xanthomonas campestris | - Branched homopolysaccharide. - Helical structure, non-allergenic, with slow dissolution rate. - Thermo-induced behavior of its sol–gel phase transition. - Good stability at high temperatures and pH due to a dimeric or double-stranded structure. - Pseudo-plastic and non-Newtonian fluid properties. | [77] |
Methods | Explanation | Ref. |
---|---|---|
Ionic interactions | By interaction mechanism between the polymer with ionic groups and some multivalent ions (di- or trivalent) of opposite charge (counter-ions). | [81,82,83] |
Hydrophobic interactions | Via a free radical mechanism, a hydrophilic monomer copolymerized with a hydrophobic comonomer. Hydrophobic interactions seem strong compared to other physical interactions, such as van der Waals bonds or hydrogen bonds). | [84] |
Crystallization (Freeze–Thawing) | After repeated freeze–thawing cycles, the polymer acquires a phase separation, which leads to microcrystal formation in its structure, creating hydrogel. Moreover, the hydrogel’s mechanical properties may be controlled by varying cycle number, time, or temperature. | [85] |
Hydrogen bonding | H-bonding occurs between functional groups of polysaccharides such as -NH2, -COOH, -SO3H, and -OH. The resulting SAPs are affected by several factors, such as polymer concentration, molar proportion, solution temperature, solvent type, etc. | [86,87,88,89] |
Complex conservation | It is an association between oppositely charged polymers (polyanionic and polycationic). Opposite charge polymers attract each other, forming insoluble and soluble complexes under diverse concentrations and pH of the polymeric solutions. | [90] |
Protein interaction | Hydrogels form by electrostatic interactions between the polysaccharide and the protein when they carry opposite electric charges. | [91] |
Coordination bonds | Adding divalent metal ions in some polymeric solutions causes coordination bonds between the biopolymer and metal ions, forming a hydrogel. | [92,93] |
Colloidal assembly | Specific polysaccharides, such as nanocellulose, have unusual self-assembling behavior. Nanocellulose particles exhibit fluid behavior in a diluted state, although they are gelled when the shear is removed. | [94] |
Methods | Explanation | Ref. | |
---|---|---|---|
(1) | Polymerization in aqueous solution | It is a reaction between neutral and ionic monomers with a multifunctional cross-linking agent in a solvent, generally water or ethanol, a water–ethanol mixture, and benzyl alcohol. The product is washed with ethanol or distilled water to eliminate unreacted reagents and oligomers. The formed gel is dried, pulverized, and sieved to achieve a specific size. | [104,105] |
(1.a)-Radical polymerization | It is also called chain-growth polymerization or cationic or anionic polymerization. The process entails four steps: initiation, propagation, chain transfer, and termination. Water is most widely used as a solvent. This method includes graft polymerization. | ||
(1.b)-Chemical reaction of functional groups | Cross-linking is performed by a reaction between functional groups (-COOH, -OH, -NH2) of hydrophilic polymers and polyfunctional cross-linking agents. As examples: (1.b.α), (1.b.β,) (1.b.γ), (1.b.δ), (1.b.ω), and (1.b.σ). | ||
1.b.α-Aldehydes: Hydrophilic polymers with (–OH) form cross-links via aldehyde cross-linking agents, such as glutaraldehyde. | [106] | ||
(1.b). β-Condensation reaction: A reaction between -OH and COOH to form polyesters or between –NH2 and –COOH to form polyamides. | [107] | ||
(1.b).γ-Addition reaction: Where higher-functional cross-linkers react with functional groups of hydrophilic polymers (such as -OH, -NH2, and COOH). | [108] | ||
(1.b).δ-Schiff-base reaction: Occurs between aldehyde and amine groups. The gelation kinetics and the physical properties of SAP can be modified by changing the ratio of those groups. | [109,110,111,112] | ||
(1.b).ω-Epoxide-based cross-linking: Epoxide polymers and cross-linking agents (such as epichlorohydrin) are water-soluble compounds highly reactive to nucleophile groups of polysaccharides (-OH and -NH2). | [99,113] | ||
(1.b).σ-Click chemistry: Consists of three classical click reactions: Cu2+-catalyzed thiol-alkene addition, azide-alkyne (3 + 2) cycloaddition, and furan-maleimide (4 + 2) Diels–Alder cycloaddition. | [114] | ||
(1.c)-Enzyme-induced cross-linking | The SAP’s preparation is induced by enzymes (such as transglutaminase, tyrosinase, horseradish peroxidase, and lysyl oxidase) acting as a catalyst in cross-linking or forming covalent bonds with polysaccharide chains without interfering with other polymers’ functional groups. | [115] | |
(2) | Inverse-phase suspension polymerization | It involves two phases: - The organic phase consists of a non-polar solvent (such as toluene or n-hexane) and a stabilizer (to maintain the dispersion); - The aqueous phase consists of monomers, initiators, and cross-linker. The produced SAPs are obtained as powder or beads with desired sizes. | [116] |
(3) | Irradiation polymerization | Irradiation is applied as an initiator to generate radicals’ formation on the polysaccharide chains (via homolytic splitting of the C-H bonds) for the cross-linkage action. It depends on various parameters, including radiation dose, the medium’s polymer concentration, and the presence of oxygen. The advantage of irradiation compared to the chemical initiation techniques is that the resulting hydrogel is relatively pure since no initiator is implicated. Commonly used methods are glow discharge [117], gamma-ray irradiation [118], electron beam irradiation [119], microwave irradiation, and ultrasonication [120]. | [121,122,123] |
(4) | Photo-polymerization | The cross-linking process uses a light corresponding to the absorption wavelength (180–220 nm) of the polysaccharide’s group and the cross-linking agent. | [124] |
Materials | Synthesis | Results | Ref. |
---|---|---|---|
- Carboxymethyl cellulose (CMC). - Starch aldehydes (CS and PS, prepared by periodate oxidation (with NaIO4) of corn and potato starch). - Citric acid (CA). | Cross-linking reaction between CMC (1 g) and starch aldehyde (1 g) by CA (10% and 20% molar ratio). | - Application: water reservoir. - Porous structure with a large specific surface. - The highest equilibrium swelling ratios were 87.0 g/g and 80.6 g/g for CS20-CA0 and PS30-CA0, depending on the starch’s source and the cross-linking density. | [165] |
- Sodium alginate (SA) (oxidized with NaIO4). - Chitosan oligosaccharide (COS). - Zinc oxide nanoparticles (ZnO NPs). | - SA + COS with different molar ratios (3:1, 2:1, 1:1, 1:2, and 1:3) to synthesize SA-COS hydrogels. - SA-COS-ZnO: mixing ZnO NPs (dispersed in 2 mg/mL of SA) with COS solution. | - Application: Wound healing. - 3D porous structure (80%). - Hydrogels provided a humid and antibacterial environment for wound healing, with good mechanical properties and swelling degree (maximum 150%). - 18% of Zn2+ was released in 24 h and 60% was released in 150 h. - Antibacterial activity followed the order SA-COS < SA-COS-ZnO, due to ZnO. | [166] |
- Cellulose (pristine eucalyptus residues (PERs) or treated eucalyptus residues (TERs)). - Gelatin (G). - Glutaraldehyde (H) as a cross-linking agent. | - SAP GH: G cross-linked with H. - GH-PER, GH-TER (SAP composites) where TER and PER (1, 3, 5%) act as a filler (fibers). | - Application: Cr(VI) adsorption from contaminated water. - Fibers improved thermal stability, rigidity, and cross-linking density. - Maximum swelling capacity: 466.1%. - The swelling capacity followed the order: GH-PER1 (497.4%) > GH > GH-PER3 > GH-PER5 and GH > GH-TER1 (413.9%) > GH-TER3 > GH-TER5. - The adsorption capacity followed the order: GH-TER5 (13.3) > GH-PER3, GH-PER5, GH-TER3 (12.4) > GH (12.3) > GH-TER1 (12.2) > GH-PER1 (12). | [167] |
- Cellulose. - Chitosan. - LiBr (solvent). | Via a codissolution and regeneration procedure in LiBr, with different ratios of cellulose and chitosan | - Application: removal of heavy metals (Cu2+, Zn2+, and Co2+) from water. - Chitosan introduced functionality for metal adsorption, increased the specific surface area, and enhanced the mechanical strength (due to H-bonds) of the composite SAP. - Mesoporous structure (27–300 Å). - Metal adsorption followed the order: Cu2+ > Zn2+ > Co2+. | [168] |
- N-carboxymethyl chitosan (CMC). - Alginate (Alg). - Calcium chloride (CaCl2) as a cross-linking agent. | Dual-physical cross-linking via both electrostatic interaction and divalent chelation by Ca2+ cations with various compositions. | - Application: Cell proliferation and wound healing. - Enhanced mechanical properties. - 3D network structure with irregular pores (dimeter = 50–100 µm). - CMC-Alg-4, prepared with 1 g of CMC, 40 mg of Alg, and 32 mg of CaCl2, exhibited better results in terms of water retention ability, rheology, the release rate of EGF, cell proliferation efficiencies, and wound healing. | [169] |
- Chitosan (CS). - Carboxymethyl cellulose (CMC). - Graphene oxide (GO) as a cross-linking agent. - Potassium persulfate (KPS) as initiator. | CS (0.5 g) and CMC (0.5 g) are chemically cross-linked by GO, which was previously functionalized with vinyl groups via grafting with VTES. | - Application: Adsorption of dyes (cationic MB and anionic MO) from contaminated water. - Adsorption of 82% dye (from 50 mg/L of MO solution) with 0.4 g/L of the hydrogel at pH 3 and 99% dye (from 50 mg/L of MB solution) with 0.4 g/L of the hydrogel at pH 7. - Maximum adsorption capacities: 404.52 mg/g for MO and 655.98 mg/g for MB. | [170] |
- Cellulose nanofibers (CNFs). - Starch (ST). - Poly (acrylic acid) (PAA). - Potassium persulfate (KPS) as initiator. - MBA as a cross-linking agent. | CNFs incorporated in different compositions in ST-g-PAA, previously prepared by graft polymerization in the presence of KPS and MBA. | - Application: Removal of Cu2+ ions from water. - Cu2+ adsorption capacity of SAPs was improved after the incorporation of NFCs. - Maximum Cu2+ uptake was 0.957 g/g in 0.6 g/L Cu2+ solution at pH (5). | [171] |
- Magnetic nanocellulose (m-CNCs) (coprecipitated from cellulose nanocrystals. - Alginate (Alg). - CaCl2 for physical cross-linking. | m-CNCs were incorporated into alginate-based hydrogel beads, physically cross-linked with CaCl2. | - Application: Drug delivery (ibuprofen). - The highest swelling degrees were 2477% in PBS medium, 515% in SGF, and 665% in water. - m-CNCs improved the mechanical toughness, increased the swelling rates, and decreased the rate of drug release of the SAPs. | [172] |
- 2,3-dialdehyde cellulose (DAC) (by periodate oxidation of nanocellulose). - Chitosan (CS). | Cross-linking between DAC and CS (dissolved in HCl) with different compositions at three different reaction temperatures (22.5, 40, and 80 °C). | - Application: Adsorption of Congo red dye. - The SAPs had a porous structure and showed good thermal and morphological stability, with a fast and high adsorption rate at pH 2 (a maximum of 100%) and excellent desorption properties at pH 12. | [173] |
- Cellulose. - Chitosan. - Dialdehyde cellulose (DAC) as a cross-linking agent. - LiOH and urea as solvents. | Via dissolution–regeneration by LiOH/urea aqueous solution, before cross-linking reaction with DAC (Schiff base reaction with chitosan), with various compositions. | - Application: Adsorption of bovine serum albumin (BSA). - Good thermal stability, with higher stability in pH 2–9 over 21 days. - The higher BSA adsorption was about 470 mg/g at pH 5.5, due to the significant electrostatic interactions between protonated amino groups of chitosan and the dissociated carboxyl groups of BSA. | [174] |
SAP Based on | Hydrogels | Gel Content Variation | Ref. |
---|---|---|---|
- Chitosan (CS) - Na-alginate (Alg) - Polyacrylamide (PAAm) | Via γ-rays: - PAAm-Alg - PAAm-Alg-CS - PAAm-CS; with several copolymer compositions. | - For PAAm-Alg: Any increase in Alg content or decrease in irradiation dose causes a reduction of the gel content. - For PAAm-CS: The gel content decreases with an increase in irradiation dose or chitosan content. - For PAAm-Alg-CS: At lower irradiation doses, similar behavior of PAAm-Alg was obtained. The gel content decreases in this order: PAAm-Alg > PAAm-Alg-CS > PAAm-CS. | [191] |
- Sodium carboxymethyl cellulose (NaCMC) - FeCl3 | Using different percentages of the reagents. | When the concentration of NaCMC increases, the cross-linking density increases, so the gel content increases. NaCMC-12, prepared by NaCMC (7%) and FeCl3 (10%), presents the full gel content. | [192] |
Effect of: | Swelling Behavior | Ref. |
---|---|---|
Salt concentration | Increasing the ionic concentration reduces the mobile ion concentration between the hydrogel network and the external medium (i.e., osmotic swelling pressure), reducing the hydrogel volume and the gel shrinks. As a result, the swelling rate decreases. | [182,191,222,230,231] |
Charge | Hydrogels with carboxylic moieties have varying swelling capacities in mono-, di-, and trivalent cation solutions. The hydrogel swelling is compared in monovalent (NaCl), divalent (CaCl2), and trivalent (AlCl3) ions at 0.5 M in solution at 25 °C. Multivalent cations (Ca2+ and Al3+) create coordination complexes with -COO− groups of SAP. These interactions serve as further cross-linkages in the gel network, significantly reducing the water absorption rate. In fact, trivalent cations reduce the absorption capacity more than bivalent cations, which are more effective than monovalent cations. So, when the cation charge increases (Na+ < Ca2+ < Al3+), the absorption capacity decreases following the order Al3+ < Ca2+ < Na+. | |
Ion size | The SAP’s capacity to absorb water increases with decreasing radius of the cation of the same valence. The results of this factor are useful because as the size of the ions in the swelling media increases (e.g., Na+ < K+ and Mg2+ < Ca2+), the swelling capacity of the hydrogel decreases (following the order Na+ > K+ and Mg2+ > Ca2+), due to the difficult penetration of the ions into the SAP. |
Polysaccharides Used in Preparing Adsorbent Hydrogels | Heavy Metals or Dyes | Maximum Adsorption Capacity in mg/g | Ref. | |
---|---|---|---|---|
Heavy metals | Chitosan | Cu(II), Cr(VI) | 116.6 and 107.5, respectively | [250] |
Chitosan | Cu(II) | 185.5 | [251] | |
Chitosan/Alginate | Pb(II), Cd(II), and Cu(II) | 176.5, 81.25, and 70.83, respectively | [252] | |
Chitosan | Cr(VI) | 102.56 | [253] | |
Cellulose | Pb2+ | 558.7 | [254] | |
Cellulose | Cu(II), Ni(II), Zn(II), Pb(II), and Cr(III) | 253.8, 112.2, 148.4, 248.2, and 30.4, respectively | [255] | |
Cellulose | Ni(II) and Cu(II) | 112.74 and 109.77, respectively | [256] | |
Chitosan/Starch | Cu2+, Ni2+, Co2+ | 100.6, 83.25, and 74.01, respectively | [49] | |
Chitosan/Glucan | Pb(II), Cu(II), Cd(II), Co(II), and Ni(II) | 395, 342, 269, 232, and 184, respectively | [139] | |
Cellulose | Cr(VI) | 13.3 | [167] | |
Cellulose/Chitosan | Cu2+, Zn2+, Co2+ | Cu2+ > Zn2+ > Co2+, where Cu2+ (94) | [168] | |
Cellulose nanofibers/Starch | Cu2+ | 957 | [171] | |
Alginate | Cu2+, Cd2+ | 13.38 and 9.54, respectively | [257] | |
Alginate | Pb2+ | 234.8 | [258] | |
Guar gum | Cr6+ | 101 | [259] | |
Pectin | Pb2+ | 390.9 | [260] | |
Salecan | Cd2+ | 421.5 | [261] | |
κ-Carrageenan | Hg2+ | 229.9 | [262] | |
Dyes | Chitosan | Methyl orange | 1060 | [263] |
Chitosan | Methylene blue | 20.408 | [264] | |
Chitosan/β-Cyclodextrin | Reactive blue 49 | 498 | [265] | |
Starch | Methylene blue | 2276 | [266] | |
Starch | Methylene blue | 2225 | [267] | |
Alginate/Chitosan | Methylene blue | 137.2 | [268] | |
Xanthan gum | Crystal violet | 1567 | [269] | |
Agarose/κ-Carrageenan | Methylene blue | 242.3 | [270] | |
Heavy metals and dyes | Cellulose | Cu(II), methylene blue | 85 and 138, respectively | [128] |
Chitosan | Cd(II), methylene blue | 90.038 and 23.478, respectively | [141] | |
Starch | Cr(VI), naproxen drug | 420.13 and 309.82, respectively | [157] | |
Starch | Co2+, basic violet | 350 and 600, respectively | [271] | |
Pectin | Methyl violet, methylene blue, Pb(II), Cu(II), Co(II), and Zn(II) | 265.49, 137.43, 54.86, 53.86, 51.72, and 50.01, respectively | [187] | |
Other pollutants | Alginate | Phenol | 994 | [272] |
Cellulose | Tetracycline | 44.9 | [273] | |
Alginate | Phosphate | 16.4 | [274] | |
Konjac glucomannan | Phosphate | 16.1 | [275] | |
Chitosan | Ciprofloxacin | 82 | [276] | |
Agarose | Ofloxacin | 581.4 | [277] | |
Xanthan gum | Bisphenol A | 458 | [278] |
Polysaccharides Used in Hydrogel Preparation | Applications | Ref. | |
---|---|---|---|
Drug delivery | Cellulose | Drug delivery | [282] |
Carboxymethyl cellulose | Drug release in cancer therapy | [125] | |
Carboxymethyl cellulose | Drug delivery | [130] | |
Chitosan/Dialdehyde starch | Betamethasone ocular delivery | [283] | |
Carboxymethyl chitosan/Alginate | Lidocaine delivery | [284] | |
Chitosan/Pullulan | Ibuprofen, bacitracin, and neomycin delivery | [285] | |
Nanocellulose/Alginate | Ibuprofen delivery | [172] | |
Wound dressing | Carboxymethyl cellulose | Dressing and skin replacement | [204] |
Sodium alginate/Chitosan | Wound healing | [166] | |
Carboxymethyl cellulose/Alginate | Cell proliferation and wound healing | [169] | |
Carboxymethyl chitosan/Methacrylate sodium alginate | Skin wound healing | [286] | |
Tissue engineering | Alginate | Meniscal repair | [181] |
Alginate | Cartilage tissue engineering | [287] | |
Cellulose nanofibers/Chitosan | Intervertebral disc annulus fibrosus tissue repair | [288] | |
Chitosan | Cartilage tissue engineering | [289] |
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Berradi, A.; Aziz, F.; Achaby, M.E.; Ouazzani, N.; Mandi, L. A Comprehensive Review of Polysaccharide-Based Hydrogels as Promising Biomaterials. Polymers 2023, 15, 2908. https://doi.org/10.3390/polym15132908
Berradi A, Aziz F, Achaby ME, Ouazzani N, Mandi L. A Comprehensive Review of Polysaccharide-Based Hydrogels as Promising Biomaterials. Polymers. 2023; 15(13):2908. https://doi.org/10.3390/polym15132908
Chicago/Turabian StyleBerradi, Achraf, Faissal Aziz, Mounir El Achaby, Naaila Ouazzani, and Laila Mandi. 2023. "A Comprehensive Review of Polysaccharide-Based Hydrogels as Promising Biomaterials" Polymers 15, no. 13: 2908. https://doi.org/10.3390/polym15132908