Journal of Polymers and the Environment

https://doi.org/10.1007/s10924-023-02796-z

REVIEW

Production of Polymer Hydrogel Composites and Their Applications

Marwa M. El Sayed1

Accepted: 8 February 2023

© The Author(s) 2023

Abstract
Hydrogels are three-dimensional cross-linked stable network insoluble in water, which gives them a remarkable capacity to
absorb both water and biological fluids. Hydrogel has been synthesized from natural or synthetic polymers and/or mono-
mers, which have made tremendous advancements in many different applications. Composite hydrogel is a type of hydrogel
prepared by grafting hydrophilic groups, such as hydroxyl (–OH), carboxylic acid (–COOH), imide (–CONH), sulfonic acid
(–SO3H), amine (–NH2), and amide (–CONH2), into the polymer chain’s backbone and adding some additives such as kaolin,
zeolite, or even different types of nanoparticles. Whereas the polymeric composite hydrogels exhibit stimuli for different
properties such as pH, temperature, or light, which may affect swelling, mechanical properties, and self-healing, which in turn
play vital roles in different areas. Hence, numerous efforts have been made to synthesize polymer-based composited hydrogels
via physical or chemical crosslinking techniques to enhance their physiochemical, biological, and many other properties.
Many researchers are currently paying attention to hydrogels and their applications, including wastewater treatment and
purification, medical and biomedical applications, agricultural applications, and many other industrial applications. The aim
of this review is to summarize the classification of composite hydrogels based on their chemical and physical crosslinking
techniques, in addition to the different polymers and additives used to prepare composite hydrogels. Furthermore, the impact
of hydrogel on health and the environment has been discussed. Other significant issues were also presented, including the
challenges that face hydrogel production and application, which have been discussed.

Keywords  Applications · Composite · Hydrogel · Polymer

Introduction are compounded in manufacturing with organic or inorganic

Hydrogel refers to a water-insoluble polymeric network with
a high-water absorption capacity. Wichterle and Lim made
the initial suggestion in the 1960s [1]. Additionally, the
hydrogel is a network of crosslinked, chain-based macromo-
lecular polymer gel. Hydrogels can have different 2D or 3D
architectures due to chemical or physical cross-linking [2, 3].
Due to their high strength-to-density ratio, processing
simplicity, and comparatively low manufacturing energy
requirements, polymers have experienced the biggest devel-
opment in uses for hydrogel synthesis during the past few
decades [4]. However, most polymers are neither useful nor
strong enough mechanically, particularly in terms of electri-
cal and thermal conductivity [5]. More than 95% of polymers
* Marwa M. El Sayed
dr.marwameid@gmail.com
1
Chemical Engineering and Pilot Plant Department, National
Research Centre, Cairo, Egypt
additives to generate polymer-based composites, which are
designed to get around these constraints. In the first genera-
tion of hydrogels, they were often made of a single polymer
and frequently had a single purpose [6]. While, after a period
of time new hydrogels composed of more than one polymer
and monomer that which called composite hydrogels have
been synthesized. This composite hydrogel can display a
variety of properties because it is made up of individual
components. Where, by combining various polymers, com-
posite hydrogels can carry out different functions [2, 7]. A
composite polymer hydrogel is created using various neutral,
cationic, and anionic monomers. The mechanical and other
different properties of composite hydrogels as well as their
applications have been investigated, and several excellent
reviews have been published [8].
Natural polymer-based hydrogels offer benefits as core
materials used in the hydrogel production due to their
biocompatibility, biodegradability, tunability, molecular
binding capacity, and bioactive characteristics [9, 10].An

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Example of natural polymers used in the hydrogel synthesis
are the polysaccharides, which are found in nature. Polysac-
charides are a source of hydrogel production. Alginate, col-
lagen, and gelatin, for instance, have all been utilized in the
manufacture of biomaterials [11]. Synthetic polymers have
great water absorption and excellent mechanical capabilities.
Synthetic materials used in the preparation of various types
of hydrogels include poly(ethylene) glycol (PEG), polycap-
rolactone (PCL), and polylactic acid (PLA) [6]. Because
of their biodegradability and potential toxicity, polymer
hydrogels have been limited in their application for various
sustainability and safety concerns, making natural-source
hydrogels more advantageous.
Many types of monomers have been used in the hydro-
gel synthesis such as acrylic acid (AA) and 2-acrylamide-
2-methyl-1-propanesulfonic acid (AMPS) have been used to
create different hydrogels [12]. As they all have the advan-
tage of conspicuous film-formability, a high swelling rate,
sustainability, and biocompatibility, they all exhibit different
swelling behaviors in response to external stimuli such as
pH [13], ionic strength, molecular species, swelling medium
composition, temperature, and pressure environment. They
are produced from hydrophilic monomers using either chain
growth polymerization (ex. free radical polymerization) or
step growth polymerization processes (ex. condensation and
addition polymerization), along with a useful crosslinker to
aid in the development of networks. By using molecular
entanglements or chemical crosslinking, homopolymers or
copolymers, whether synthetic or natural, are employed to
create three-dimensional networks. Natural polymer hydro-
gels and synthetic polymer hydrogels can be distinguished
according to the substance used to synthesize the hydrogels
[14].
Hydrogel can be used in a variety of industries, including
slow-release fertilizers [15, 16], soil amendments [17], drug
delivery systems [18], tissue engineering [6], wound dress-
ings, personal hygiene products [16], cosmetics, textiles, and
wastewater treatment [19]. The current review provides a
broad discussion and analysis of advanced hydrogel prepara-
tion and application status aspects, including hydrogel clas-
sifications, polymer sources, the most advanced and new
applications, and some economics of hydrogel production
[20].
Classifications of Composite Hydrogel
Hydrogels are often classified according to their configura-
tion, physical appearance, polymer composition, method of
crosslinking, electrical charge of the network, and sources.
Figure 1 summarizes how hydrogels are classified.
For example, according to the hydrogel source, hydrogels
are either natural, synthetic, or hybrid, depending on the
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Journal of Polymers and the Environment
source of the polymer network [21]. These polymer hydro-
gels are crosslinked as copolymeric and multi-polymeric
networks [22]. Additionally, the single, double, and multi-
polymers are crosslinked either chemically or physically,
resulting in chemical and physical hydrogels that are single,
double, and multi-polymers [14].
Hydrogels can also be divided into crystalline, semi-
crystalline, and non-crystalline types based on their arrange-
ment, physical structure, and chemical makeup. Importantly,
crystalline and amorphous materials are both parts of semi-
crystalline materials [11].
Classification According to Parent Chain Sources
Hydrophilic monomers that form double bonds during
polymerization are used to create hydrogel from a polymer
substrate. Natural, synthetic, or a combination of natural and
synthetic polymers make up polymeric hydrogels. Different
monomer types offer the hydrogel with various mechanical,
salt-tolerance, and water-retention qualities [22].
Natural Polymers
Starch (St)  Starch (St) is a natural polysaccharide made up
of anhydro glucose units that are linked together. Each of
these units has three hydroxyl groups. Starch granules con-
tain amylose and amylopectin [23].
Chitosan (CS)  Chitosan (CS) is a linear polysaccharide com-
posed of -(1-4)-linked 2-amino-2-deoxy-d-glucose (d-glu-
cosamine) and 2-acetamido-2-deoxy-d-glucose (N-acetyl-
d-glucosamine) units. It is biocompatible and biodegradable,
and its degradation products are non-toxic [24–26].
Alginate (Alg) Alginate (Alg) is a linear polysaccharide
synthesized using brown algae in addition to some bacteria.
It is composed of 4-linked d-mannuronic acid (M) and its
5-epimer, 4-linked R-Lguluronic acid (G) [27].
Collagen  The major extracellular matrix protein, colla-
gen, is found in the skin, ligaments, tendons, blood vessels,
bones, and cartilage, among other connective tissues in the
body. The three most prevalent forms of collagen, types I,
II, and III, are among the many that have been found and
characterized. Due to its significant presence in live human
connective tissues and ease of extraction and purification
from the tissue, type I collagen is the most significant and
widely utilized kind of collagen in the preparation of hydro-
gels [28].
Cellulose  The most widely used, affordable, and biodegrad-
able substance is cellulose, which is generated in large quan-
tities from various agricultural wastes, as indicated in Fig. 2.
Journal of Polymers and the Environment

Fig. 1  Classification of hydrogels based on the different properties

Fig. 2  Sources of cellulose for hydrogel production [29]

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 Journal of Polymers and the Environment

The primary component of plants and natural fibers like linen
and cotton is cellulose, a polymer of glucose. The 1,4-gly-
cosidic connections that connect the glucose units are what
cause natural cellulose's high crystallinity and insolubility
in water and other common solvents. Native cellulose may
be dissolved in solvents like N-methylmorpholine-N-oxide
monohydrate or ionic liquids to create hydrogels, which can
then be coagulated with water [16].
Hyaluronic Acid (HA)  N-acetylglucosamine and glucuronic
acid make up the widely distributed linear polysaccharide
known as HA, which is present in connective tissue [30].
A naturally occurring biopolymer, hyaluronic acid serves
a variety of purposes in the body, including wound heal-
ing, cell migration, and cell signaling. Hyaluronic acid has
played a significant role in biomedical research because of
its adaptability and has been used in a variety of sectors,
including tissue engineering and the treatment of cancer,
through a variety of various forms. It has a high viscoe-
lasticity, is biocompatible, and doesn't cause an immune
response [31].
A list of some trustworthy natural polymers utilized in the
manufacture of hydrogels is shown in Table 1.
These polymers eventually disintegrate into the respective
hydroxyl acids as harmless degradation products by hydro-
lytic breakage of their ester linkages [14].
Poly(ethylene glycol) (PEG)  For the hydrogel crosslinking
process, PEG is easily reacted with functional groups such
as acrylate, thiol, epoxy, carboxylic acid, and amine. The
functionalized end groups in PEG precursors can help the
hydrogels' biodegradation even when the PEG backbone
lacks a biodegradable component. Hydrogels used in medi-
cal applications have already been improved in terms of
their biocompatibility and mechanical integrity using PEG
hydrogels [41].
PVA  Due to its permeability and rubber-elastic physical
characteristics (compressive, shear, and tensile modulus), as
well as the high-water content, Polyvinyl alcohol (PVA), a
hydrophilic polymer, has been utilized to create hydrogels
for the replacement of injured cartilage [42].
Classification According to Crosslinking
Chemically Crosslinking

Synthetic Polymers By combining chemical crosslinkers with polymers and cre-

The most well-known synthetic and biodegradable polymers
utilized in the production of hydrogels are those contain-
ing poly-hydroxyl acids, such as Polyethylene glycol (PEG),
poly(glycolide-co-lactide), polyvinyl alcohol, poly(n-iso-
propylacrylamide), poly(l-lactic acid), and poly(l-lactide).
ating covalent bonds, chemically crosslinked hydrogels are
created. Since it does not dissolve in water without rupturing
covalent bonds, this type of hydrogel is stable and long-last-
ing [43]. A completely cross-linked hydrogel has less design
flexibility since it is challenging to decouple elements like
gelation time, inward network pore size, functionalization,

Table1  Examples of natural polymers used in hydrogel synthesis

Polymer Monomer Initiator Crosslinker Reaction conditions Aim Refs.
o
Time h Temp C

Chitosan Acrylic acid APS* MBA 4 50 Medical App [32]

Chitosan Acrylic acid – VTMS 5 65 Agricultural [33]
Chitosan Acrylic acid APS MBA* – 60 Oil separation [34]
Chitosan Acrylamide – – 120 50 Dye removal [24, 26]
Starch – – – 0.25 100 Wound Dressing [35]
Polyvinyl alcohol
Starch Acrylonitrile Microwave 30–15-S – – [36]
Starch Acrylonitrile CAN* MBA – 95 Agricultural [37]
Starch Acrylamide Ultrasonic heating 2 – Enhanced water-Retention [38]
(400 W 40 kHz)
CAN* MBA
Alginate Acrylic acid APS MBA 0.5 50 Dye removal [39]
Carboxy methyl cellulose Acrylic acid APS MBA 2 50 Heavy metals Removal [40]
and Acryla-
mide

APS ammonium per sulphate, CAN ceric ammonium nitrate, MBA N,N′-methylene bisacrylamide, VTMS vinyl tri-methoxysilane

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Journal of Polymers and the Environment
and degradation time. The different types of chemical cross-
links and polymerization techniques are shown in Fig. 3.
Unexpectedly, by combining physical and chemical
crosslinking network creation through electrostatic contact,
a novel dual-network hydrogel is produced. Keep in mind
that free radical polymerization may be used to create poly-
mer hydrogels from synthetic, semi-synthetic, and natural
hydrophilic polymers [44].
Chain Growth Polymerization “Free Radical Polymeriza‑
tion”  The best technique for making hydrogels based on dif-
ferent monomers, such as acrylates, amides, and vinyl lac-
tams, is free radical polymerization. Additionally, it may be
utilized to create hydrogels made from natural polymers that
contain the right functional groups or have been functional-
ized with radically polymerizable groups. Radical polym-
erizations are fast and relatively impervious to impurities;
they can be performed as bulk, solution (also in water),
emulsion, suspension, or precipitation polymerization [11].
A series of experiments have been conducted to demon-
strate the free radical polymerization process. In general,
there are three stages: (1) initiation, in which initiators
decompose at high temperatures and produce free radicals;
(2) propagation, in which active sites attack vinyl monomers
to copolymerize and complete the grafting polymerization;
and (3) termination, in which a 3D network structure is cre-
ated with the help of cross-linkers [12]. It should be noted
that in the reaction systems, monomer cross-linking, and
self-polymerization can both occur at the same time. For
instance, ethylene glycol di-methacrylate (EGDMA) was
Fig. 3  Various techniques of chemical cross-linkages polymerization
used as a crosslinking agent, and benzoyl peroxide was
used as a reaction initiator to create PVA-based hydrogels
by chemical crosslinking with methacrylic acid in aqueous
solutions [45].
Polymer hydrogels have been made from vinyl mono-
mers like N-vinyl indole derivatives, N-vinyl pyrrolidone,
and N-vinyl formamide through a process called controlled
radical polymerization [46].
For the crosslinking to begin when light is applied during
photo-polymerization, photo initiators must be introduced to
the polymer solution. In contrast, catalyst-based free radical
polymerization causes the generation of free radicals and
then polymerization to crosslink the network. Examples of
such catalysts are ammonium persulfate (APS) and tetra-
methylethylenediamine (TEMED) [11].
According to the above-mentioned method, different ini-
tiators and monomers are poured into the aqueous solution.
Also, covalent bonds can be constructed between vinyl mon-
omers. Many published articles related to superabsorbent
hydrogels are based on using hydrophilic monomers. Free
radicals can be generated to initiate the polymerization reac-
tion by chemical induction systems, for instance, ultraviolet
(UV) photopolymerization, thermal initiators (e.g., ammo-
nium persulfate and benzoyl peroxide), redox-induced sys-
tems ­(Na2SO3 and bisulfite), and cerium nitrate [40].
Step Growth Polymerization  Condensation polymerization
TEMED and N-3-dimethylaminopropyl-N-ethyl carbodi-
imide (EDC), two polyfunctional crosslinking agents, are
gradually mixed during condensation and addition polym-
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Fig. 4  A model for solution polymerization reactor [43]
Table 2  Physically crosslinked No Polymer hydrogel
polymer hydrogels [50]
1 Calcium Alginate
2 Chitosan-Alginate
3 Hyaluronan
4 PVA- Alginate
5 Sodium CMV- PVA
erization [47]. In condensation polymerization, a water mol-
ecule is released as a result of the bonds formed between the
polymers. Polyesters and polyamides may be synthesized
using condensation polymerization, and polymer hydrogels
can also be synthesized through similar processes. To create
composite polymer hydrogels, different polymers (natural
or synthetic) can be crosslinked using one of the following
crosslinkers: 1,6-hexamethylene diisocyanate, divinyl sul-
fone, or 1,6-hexane dibromide [48].
Solution Polymerization The reactants are dissolved in
water at concentrations between 10 and 70% during the solu-
tion polymerization process. Before or after the polymeriza-
tion, groups like carboxylic acid in the product are partly
neutralized. In this process, the initiation is often accom-
plished chemically with a free-radical azo or peroxide ther-
mal dissociative species or by the interaction of a reducing
agent with an oxidizing agent (redox system) [43]. However,
this approach is preferable at both laboratory and industrial
scales because of its quick process, lower cost, and accept-
able swelling qualities. A model for the solution polymeriza-
tion reactor is shown in Fig. 4.
Irradiation Polymerization  Another technique used to syn-
thesize polymer-based hydrogel is the irradiation polymeri-
zation technique. Hydroxyl groups detach from polymeric
chains when aqueous solutions of polymers are subjected
to gamma or electron beam radiation. These -OH groups
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Journal of Polymers and the Environment
can then attack polymer chains, resulting in the formation
of more micro-radicals. As these micro-radicals mix on
various polymer chains, covalent linkages are produced in a
crosslinked form [2, 49].
Polysaccharides, PVA, PEG, and PAA were discov-
ered to be polymers for irradiation-based crosslinking. It
was discovered that during irradiation, polysaccharides
with carboxylic acid groups participated in a crosslinking
process [50]. For example, a grafted copolymer derived
from gum ghatti (Gg) and acrylic acid was synthesized by
gamma radiation [51]. In order to create composite poly-
mer hydrogels, a grafting process was carried out in the
presence of a low concentration of potassium persulfate
initiator and MBA crosslinker using microwave (MW) or
ultraviolet (UV) irradiation techniques [52]. In another
study, branched polyethyleneimine (PEI)-grafted GO-
Crosslinking type Physical method Refs.
Ion-polymer interaction Mixing and stirring [54]
Hydrophobic interaction Mixing and stirring [55]
Hydrogen bonding Freeze-thawing [18]
Polymer–polymer complexation Freeze-thawing [50]
Hydrogen bonding Freeze-thawing [56]
AgNPs antibacterial nanocomposites (PEI-GO-AgNPs)
were integrated using microwave irradiation to develop a
slow-release antibacterial hydrogel for a more stable and
sustained antibacterial effect. An antibacterial mechanism
has been proposed according to the experimental observa-
tion [53].
Physically Crosslinking
Physically crosslinked polymer hydrogels are formed
through non-covalent crosslinks [11]. This is usually
achieved via diverse physical processes such as complexa-
tion (e.g., ion–polymer and polymer–polymer), hydropho-
bic organization, chain aggregation, crystallization, and
hydrogen bonding as illustrated in Table 2. Amphiphilic
block and graft copolymers assemble their chains in such a
way that ordered structures are built through the aggrega-
tion of hydrophobic segments of the polymers. Because
of hydrophobic interactions, isopropyl groups (for exam-
ple, in poly(N-isopropyl acrylamide)) can be physically
crosslinked. Physically crosslinked polymer hydrogels can
also be made from polysaccharides such as dextran, chi-
tosan, and carboxymethyl curdlan via hydrophobic organi-
zation [50].
Journal of Polymers and the Environment
Fig. 5  Ionic interaction [29]
Fig. 6  H-bonding [29]
Table  2 illustrate different polysaccharides used as
substrate for the polymer hydrogel synthesis via physical
crosslinking mechanism [50].
Ionic Interactions  Hydrogels can be crosslinked via ionic
interactions under mild conditions at physiological pH
and room temperature. Ionic groups in the polymer are not
required for this cross-linking reaction. Stronger hydrogel
is produced by metallic ions. An excellent illustration of
a polymer that may be crosslinked by ionic interactions is
alginate. Alginate is a naturally occurring polysaccharide
that is crosslinked by calcium or sodium ions and yet con-
tains mannuronic and glucuronic acids [57] (Fig. 5).
Freezing/Thawing  Crystallization involves freezing/
thawing process and creates a strong and highly elastic
gel. For example, PVA hydrogels can be synthesized by
physically crosslinking through repeated freezing/thawing
methods [58].
Hydrogen Bonding  Like the development of a hydrogel
based on gelatin, hydrogen bonding between polymer
chains can also contribute to hydrogel formation. An elec-
tron-poor hydrogen atom and a functional group with a
high electronegativity combine to form a hydrogen bond.
This method of making hydrogels longer is affected by a
number of factors, such as the concentration of polymers,
the molar ratio of each polymer, the type of solvent, the
temperature of the solution, and the degree to which poly-
mer functions are linked [29, 58] (Fig. 6).
Based Polymer for Composites Hydrogel
Depending on the base polymers used to make the hydro-
gel substrate, different types of functional groups like car-
boxylic acid, amine, hydroxyl, amidoxime, and sulfonic
acid groups can be added. This can improve the ability to
absorb and many other properties [11].
For a variety of uses, hydrogel-composite preparations
have recently attracted a lot of attention. There are numer-
ous drawbacks to synthetic hydrogels, including their high
production costs and latent toxicity [14]. Researchers have
created hydrogel composite materials made of natural,
inexpensive, nontoxic, and biodegradable components to
address these main limitations relating to cost and poten-
tial environmental issues. For instance, combining the
hydrogel with a substance that has a greater adsorption
ability may dramatically increase the sorption capacity
[59]. For example, the different ways to fabricate CS-based
composite hydrogels are:
(a) Solvent evaporation method: CS is mixed with acetic
acid and spread on a plate, where it is kept drying at an
elevated temperature (around 65 °C) [60].
(b) Neutralization method: by adding CS solution through
a dropper into a dilute NaOH solution, beads are
obtained. This can be done in a water–ethanol mixture,
as chlorine does not dissolve in ethanol. The formed
beads might then be subjected to crosslinking [61].
(c) Crosslinking method: Membranes can be prepared by
spreading CS dissolved in acetic acid on a surface and
then crosslinking it with suitable crosslinking solutions
such as Glutaraldehyde or Genipin. CS beads can be
prepared by pouring drops of crosslinked chitosan solu-
tion into a coagulating agent such as NaOH or in a
non-aqueous medium such as mineral oil [62].
(d) Ionotropic gelation method: The preparation can be
accomplished by adding polyanions such as xanthan,
alginate, or carrageenan into a cationic CS solution
[63].
(e) Freeze-drying method: Hydrogels are used for tissue
engineering and regenerative medicine applications and
are produced by freezing CS solutions at extremely low
temperatures and drying them in vacuum ovens [64].
Composite hydrogels are used for tissue engineering
and regenerative medicine applications and are pro-
duced by the freeze-drying method [65].
2D GO macromolecules were used to create a PAm
composite hydrogel. The inclusion of GO enhances the
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Fig. 7  Preparation of graphene embedded PVA hydrogel and their
dye removal profile [67]
hydrogel's mechanical characteristics [50, 66]. In another
study, a composite hydrogel composed of PVA/GO was
prepared and used to remove various types of dyes, as
shown in Fig. 7 [67].
Typical Examples of Composite Hydrogel
Starch, chitosan, and alginate were used as the substrates
in composite polymer hydrogel, which was then grafted
with acrylamide using KPS and MBA as the initiator and
crosslinker, respectively [52]. The hydrogel generated (PsB-
g-Am) has the following grafting rate equation: Rg is equal
to k[Am] [­ PsB]0.5 ­[KPS]0.5.In the used concentration range,
the grafting rate is first-order dependent on the starting con-
centration of [Am] and square root dependent on the starting
concentrations of [PsB] and [KPS].
The swelling of the chitosan-grafted acrylamide/acrylic
acid hydrogel has been studied. According to statistics,
swelling increases with temperature up to 60  °C before
beginning to decrease as the temperature rises higher [68].
The swelling degree gradually increased after soaking the
hydrogel in distilled water, and the swelling degree kinetic
studies of the hydrogels were conducted at the first 8 h,
where the hydrogels' swelling degrees at the three differ-
ent temperatures are very high, as seen in Fig. 8. Swelling
values of 1.4, 1.5, 1.4, 2.3, and 0.7 g of water per g of dry
hydrogel were observed after 8 h at RT, 30, 40, 60, and 80
degrees Celsius, respectively. As seen in Fig. 8, the degree
of hydrogel swelling increased as the temperature increased.
At 60 degrees Celsius, swelling is twice as large as it is at
room temperature [68].
In another study, a novel composite hydrogel adsorbent
has been developed. The composite hydrogel is composed
of zeolite and crosslinked chitosan and has been applied to
remove acid red 88 dye from an aqueous solution [69].
Cellulose-based acrylic acid hydrogel has been created
using rice straw as the starting point. The heterogeneous
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Journal of Polymers and the Environment
Fig. 8  Swelling degree in terms of water absorbed per dry hydrogel
as a function of time and temperature [68]
reaction was used to create the cellulose-based acrylic
acid hydrogel, which has a swelling ratio greater than
300 percent [70]. For enhancing maize production in salt-
affected soil as well as in the growth promoters of maize
under water stress, a comparison between the rice straw-
based hydrogel and the commercially available acrylamide
hydrogel was explored. In general, the inclusion of hydro-
gel improves the efficiency of using water and nutrients, as
well as nutritional concentration and absorption.
The microwave (MW) and ultraviolet (UV) irradiation
have been used to graft acrylamide onto alginate and chi-
tosan. Reverse osmosis brine and salty solutions were sof-
tened using prepared polysaccharide hydrogels. Alginate
and chitosan hydrogels that were created were character-
ised (Alg-UV and Alg-MW). It was shown that swelling
increased 16.7 to 21 times more in distilled water than in
saline solutions. For grafted acrylamide hydrogels with
Alg-UV and CS-MW, respectively, the maximum obtained
swelling ratios in distilled water were 168 and 173 g/g.
Maximum calcium absorption capabilities of Alg-MW
and UV-prepared alginate and chitosan hydrogels were 54
and 34 mg/g from seawater for both dry and pre-swollen
hydrogels, respectively. Using dry alginate hydrogels and
chitosan hydrogels, respectively, the maximum magnesium
adsorption capabilities from brine were 280 and 316 mg/g
[71].
Applying the free radical polymerizing acrylic acid (AA)
in the presence of sodium alginate, a new nanocomposite
hydrogel (NCS) has been created, which was then loaded
with ­Cu2+ ions and subjected to an ammonia reaction. The
produced hydrogel was used in the dye removal process.
At a concentration of 10 mg/L and a pH of 6, it was dis-
covered that crystal violet (CV) and malachite green (MG)
had removal efficiencies of more than 96 percent. Both the
Freundlich isotherm and the pseudo-second-order kinetic
models are effective in describing the dye adsorption on the
NCS. The reusability tests revealed that after eight cycles,
around 95% of the initial adsorption was achieved [38].
Journal of Polymers and the Environment
Fig. 9  Swelling behavior of the hydrogel and NCS (a) comparison of the hydrogel and NCS for adsorption of CV (b) (T = 25 °C, the adsorbent
dosage = 0.3 g/L, pH 6, Ci = 10 mg/L, t = 2 h) [38]
Fig. 10  Adsorption capacities
of the composite hydrogels
for different heavy metals
­(Ci = 10 mg/L, pH = 4) [73]
The swelling of hydrogel and NCS in the distilled water
has been investigated (Fig. 9). The equilibrium swellings
of the hydrogel and NCS were found to be 1134 g/g and
256 g/g, respectively.
Tetra-ammine copper (II) sulphate nanoparticles' inter-
action with the hydrogel's carboxylate groups may be the
cause. As seen in Fig. 3, tetra-ammine copper (II) sulphate
can function as a cross-linker and reduce swelling capac-
ity. The hydrogel's ability to remove dye is considerably
enhanced by the addition of the nanocomplex. However,
the nanoparticles may also interact with the dye molecule
to speed up dye adsorption.
Using cost-effective modified adsorbents, carried out
batch adsorption tests for the adsorption of heavy metals.
Microwave (M) irradiation method (ACM) or ultrasonic (U)
irradiation technique have been used to create polyacrylate
hydrogels (ACU). As shown in Fig. 10, the results of equi-
librium adsorption experiments showed that the Langmuir
isotherm model is better fitted than any other model, with
maximum adsorption capacities of 84.5, 73.3, 61, and
97 mg/g for Cr, Co, Ni, and Pb, respectively. For all ions
other than Ni, the Tempkin isotherm yielded equivalent
results. The pseudo-second-order kinetic model provided
the most accurate description of the adsorption kinetics of
Cr, Co, Ni, and Pb using all the composite hydrogels. Inves-
tigations were also conducted on further mixtures of acrylic
acid salts with Egyptian kaolin (AKM and AKU) or zeolite
(AZM and AZU) [72].
Figure 10 makes it evident that adding kaolin and zeolite
to the polyacrylate hydrogel structure boosted Cr absorp-
tion (by more than 80%), notably for samples of hydrogel
that had been made using a microwave, while also margin-
ally increasing Co and Ni uptake. Additionally, Pb uptake
increased for samples treated by microwave and ultrasonic
using zeolite (27% and 3%, respectively).
For the chosen adsorbent, adsorption kinetics were inves-
tigated from 10 min to 24 h. In general, the metals adsorbed
rise quickly in the first hour and continue to rise for 3 h for
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 Journal of Polymers and the Environment

Pb and 5 h for Cr, Co, and Ni, after which the adsorption
capacity increases by no more than 2 to 5%.
This pattern could be described by the initial quick
absorption of metal ions and subsequent sluggish kinetics
into the remaining empty sites, where repulsive forces from
the initial adsorbed layer tend to reduce metal removal on
the open sites [54]. The ideal contact period is therefore set
at 3 h for Pb and 5 h for the other ions.

Composite Hydrogel Containing Nanoparticles

Due to their unique features compared to bulk materials,

nanoparticles are being used in everyday consumer goods
and appliances. Public discussion about the safety of nano-
particle technology has been sparked by this trend, and regu-
latory bodies have stepped in in several nations. By incor- Fig. 11  Schematic representation of Nano Composite Hydrogel based
porating nanoparticles into hydrogels, it may be possible to on the source of origin and application in nanotechnology [62]
overcome application problems while lowering environmen-
tal and human health hazards. Additionally, it was believed
that the creative fusion of these two very different sorts of
materials would produce a variety of property improve-
ments in addition to structural diversity. The main goal of
research on hydrogel-nanoparticle composite materials was
to improve these properties, which led to better mechanical
strength and response to stimuli [74].
Synthetic polymers are renowned for their controlled
structures and intended mechanical qualities. Nanoparticle-
encrusted polymer hydrogels have been created with appeal-
ing characteristics. The polymer hydrogels' surface area and
pore diameters are altered by highly active nanoparticles,
which improves the adsorption efficiency even further. Addi-
tionally, compared to their pure forms, the mechanical and
thermal characteristics of nanocomposite-embedded poly-
mer hydrogels were altered by a potent synergistic interac-
tion between the nanofillers and polymer matrix [8]. To pro-
vide plenty of active sites for adsorption and cross-diffusion Fig. 12  Composite hydrogel grown on agar plates after incubation
pathways for adsorbate molecules, a range of nanoparticles, with Escherichia coli and Staphylococcus aureus [41]
including ­TiO2, ZnO, Fe-nano, and Ag-nano, were investi-
gated in this respect [75]. PVA/CS/nano-zinc oxide nanocomposite hydrogels
There are different sources for NP composite hydrogel were created by the freeze-thaw method and used as
preparation. Polymers are both natural and synthetic. This wound dressings. The findings showed that longer freeze-
type of nano-composite hydrogel has many applications such thaw cycles decreased pore size, increased porosity, and
as biosensing and environmental utilities, which are sum- enhanced wound fluid absorption. Lowering the reaction
marized in Fig. 11. temperature increased the elastic modulus and tensile
strength while decreasing the elongation at break. The
biocompatibility, antibacterial properties, ability to effec-
PVA‑Based Nano‑hydrogel tively cure wounds, and toxicity of the developed HG were
all tested [76].
It has been reported that PVA polymer-based nano-hydro- To create an antibacterial hydrogel, silver nanoparticles
gels and modified PVA hydrogels employing functional (AgNPs) have been added to a PVA/bacterial cellulose
components and nanoparticles have good stimuli-responsive (BC). As seen in Fig. 12, the hydrogels had excellent anti-
biocompatibility in a variety of applications [62]. bacterial qualities and good biocompatibilities, in contrast

13
Journal of Polymers and the Environment

Table 3  A summary of reaction No Reaction rate Polymer Monomer Initiator Refs.

rate equation for grating
different vinyl monomers onto 1 0.5 0.5
Rg = ­[P] ­[M] ­[I] 0.5
Starch, Ch, Alg Am KPS [52]
polysaccharide chains [11]
2 Rg = ­[P]0.48 ­[M]0.92 ­[I]0.56 Starch AA CAN [79]
3 Rg = ­[P]0.5 ­[M]1 ­[I]0.5 Starch AN KMnO4 [80]
4 Rg = ­[P]0.52 ­[M]0.93 ­[I]0.49 Starch Am k2Cr2O7 [81]
5 Rg = ­[P]0.497 ­[M]1.185 ­[I]0.499 Starch AN KPS [35]

P polymer, M monomer, I initiator

to the PVA/BC hydrogel's lack of antibacterial activity Amount of grafted monomer

Rg (mol∕l s) =
[41]. Mm × reaction time × reaction volume

Alginate‑Based Nanohydrogel
Alginate-based nano-hydrogels, which are nanomaterials
made of gels, have been recognized for their use in regen-
erative medicine and antibacterial and antimicrobial applica-
tions [77]. Alginate has a significant function as a prodrug
and has previously been investigated for its critical role in
biomedical applications due to its non-toxicity, biocompat-
ibility, and pH sensitivity. Gum acacia copolymer-based
alginate-based nanohydrogels have been developed for their
versatile and efficient antibacterial activity. [62].
Hyaluronic‑Based Nanohydrogel
where ­Mm represents monomer molecular weight (g/g mol).
The rate of the graft polymerization (Rg) (mol/l s)
depends on the concentrations of polymer, monomer and
initiator as follows:
Rg = k[P]a [I]b [M]c (1)
where k is the graft rate constant, P, M and I denotes for
polymer, monomer and initiator, respectively: a, b and c are
constants.
A summary of reaction rate equation for grating different
vinyl monomers onto polysaccharide chains monomer has
been illustrated in Table 3

Due to its special characteristics and utilization in drug
delivery systems, HA-based nanohydrogel has demonstrated
considerable potential for nanotherapeutics and nanomedi-
cine [78]. Ketal crosslinkers used the surfactant-free one-pot
approach to create hyaluronic-based nanohydrogels [62].
Reaction Rate for Polymer Composite Hydrogel
The main task of all studying the reaction rate or in more
specified words is to study the kinetic experiments is
to assess the grafting rate via a variety of experimental
approaches. The experiments carried out to determine the
kinetics rate coefficients could be divided into two areas.
The first approach centers on the accurate measurement of
the overall polymerization rate, whereas the second one con-
centrates on the analysis of the resulting molecular weight
distributions. If all the rate coefficients for a polymerizing
system are known, it is possible to predict the kinetics of the
overall polymerization process, including the full molecular
weight distributions.
Several authors studied the kinetics of graft polymeriza-
tion of monomers onto polymer [68, 79]
The rate of graft polymerization (Rg) is estimated by the
following equation:
Super Absorbent Polymer Composite Hydrogel
By cross-linking copolymerization with different synthetic
monomers, such as vinyl monomers like NIPAM, sulfo-pro-
pyl methacrylate, potassium salt, and potassium acrylate, as
well as with natural polymers, hydrogels with high absorp-
tion capacities, or superabsorbent hydrogels (SAPs), can be
created (i.e., carboxymethyl cellulose and gelatinized corn
starch). The main substance utilized in the production of
superabsorbent hydrogels is polyacrylate. By adding linked
pores to the polymer network, "super-porous" hydrogels with
quick swelling kinetics and superabsorbent characteristics
might be created. When these hydrogels are in the xerogel
state, the pore size is hundreds of micrometers. The supera-
bsorbent hydrogels poly(N-isopropylacrylamide/acrylic
acid), or P(NIPAM/AA), were created using the free radical
polymerization process in the presence of the appropriate
cross-linker agents, initiators, and solvents [82].
In reaction to certain external stimuli like temperature,
solvent quality, pH, electric field, etc., hydrogels may show
abrupt volume changes [83]. Superabsorbent hydrogels
have many various applications such as biomedical appli-
cations, wastewater treatment and agricultural applications
[84]. When taking agricultural application as an example of
using superabsorbent hydrogels it can found that when using

13

Fig. 13  Chemical structures of conductive polymers
the right amendment and different doses of soil to hydrogel
ratio, the addition of hydrogel polymer can boost soil's abil-
ity to retain water by 50–70%. Soil bulk density can decrease
by 8–10% over time. So, super absorbent polymer hydrogels
have many advantages when applied in the agricultural flied
and these advantages may be summarized as:
– Less affected by salts
– Exhibits maximum absorbency @ temperatures (40–
50 °C), characteristic of semi-arid and arid soils.
– Absorbs water up to 400 times its dry weight.
– Low rates of soil application—1–2 kg /ha for nursery
horticultural crops; 2.5–5 kg/ ha for field crops
– Reduces leaching of herbicides and fertilizers
– Helps plants withstand prolonged moisture stress.
– Improves seed germination and seedling emergence rate.
– Reduces nursery establishment period.
– Reduces irrigation and fertigation requirements of crops.
– Promotes early and dense flowering and fruiting/ tiller-
ing.
– Delays onset of permanent wilting point
Conductive Composite Hydrogel
Electrical current is conducted across polymer chains
through p-electron conjugation in conductive hydrogels, a
subcategory of hydrogel made up of conductive polymers.
Here, the conducting polymer's atoms are linked together by
conjugated unsaturated bonding, which leads to the delocali-
zation of electrons along the polymer's conjugated bond. A
number of dopants may be easily and affordably incorpo-
rated into conducting polymers to significantly increase their
conductivity. As shown in Figure 13, polyaniline (PANI),
polypyrrole (PPy), and polythiophene (PTh) are a few exam-
ples of significant conjugated conducting polymers [1].
These conducting polymers have electrical conductivities
between ­10−6 and 1­ 0−1 S ­cm−1, which is greater than insu-
lating polymers' and lower than typical metallic conductivi-
ties. By adjusting the externally introduced dopant and its
13
Journal of Polymers and the Environment
Fig. 14  Effect of contact time on adsorption capacity of nickle (Ni)
concentration, the conducting polymer's conductivity may
be tailored. Additionally, because of their nanoscale-level
restricted dimensions, conductive polymers display distinc-
tive mechanical and optical characteristics [85].
Polyaniline (PANI) Based Conducting Hydrogels
PANI hydrogels are made of conductive PANI. These are
frequently created by polymerizing the aniline (ANI) mono-
mer inside a non-conductive gel matrix or by adding the
conductive polymer PANI to the gel matrix. ANI-to-PANI
hydrogel in-situ polymerization is commonly referred to as
a “dual network gel” [86].
In situ polymerization was used to create sodium algi-
nate-PANI (Alg-PANI) composite hydrogel for super-capac-
itors. The reinforced Alg-PANI hydrogel has an outstanding
compressive strength of 41 kPa and a strong conductivity
of ­10–3 S ­cm−1. Because it lacks adhesive and conducting
filler, Alg-PANI hydrogel is used directly as an electrode
material for supercapacitors [50].prepared an adsorptive
polyacrylonitrile-based hydrogel blend has been prepared
to examine heavy metal removal in simulated effluents incor-
porating chromium and nickel. Electrical conductivity meas-
urements indicated the presence of PANI in the polymeric
blend, which assisted in the increase in conductivity of PAN
hydrogel. Also, the effect of the contact time of the used
hydrogel and the adsorption capacity of Ni have been stud-
ied, as shown in Fig. 14. The maximum nickel adsorption
was 8 mg/g at pH 7 and 2 h of contact time [86].
Polypyrrole (PPy) Based Conducting Hydrogels
PPy-based hydrogel is another type of conductive polymer
that has been applied in the synthesis of hydrogels. PPy is
rigid and insoluble because of the delocalized p-electrons in
the polymeric chains; therefore, the synthesis of PPy-based
conductive hydrogels remains challenging.
The application of hydrogels in flexible sensors requires
high mechanical toughness and excellent self-recovery to
achieve large-range strain sensing and long-term cycling
Journal of Polymers and the Environment

Table 4  Summary of the performance of reported various ionic conductive hydrogel

Hydrogel Electrolyte Properties Refs.

P(HMA-Am) NaCl GF = 2.37, strtchability (2160%); Self-recovery, anti-fatigue, linear range (1–1000%) [85]
Agar/Pam LiCl GF = 1.8, strtchability (1600%); Self-recovery, anti-fatigue, linear range (1–1000%) [87]
PVP/PVA FeCl3 GF = 0.487, strtchability (2160%); Self-recovery, adhesion, self-healing, tensile stress (2.1 Mpa) [88]
PVA/PAA H2SO4 Self-recovery, Stretchability (2600%), linear range (0–500%) [89]
Agar/PAm NaCl GF = 2.1, strtchability (1910%); Linear range (0.5–1600%) [90]

Fig. 15  Isothermal tank for

heating monomer aqueous solu-
tion [91]

stability. Conductive hydrogels possess the additional prop- Pretreatment

erty of conductivity, which endows them with advanced
applications in actuating devices, biomedicine, and sensing.
The conductive hydrogels used in the field of strain sensors
have a conductive filler, including ionic conductors, con-
ducting nanomaterials, and conductive polymers.
Directly doping soluble inorganic salts into hydrogel is a
simple and straightforward approach to preparing conductive
hydrogel. Table 4 illustrates the performance of some ionic
conductive hydrogels [1].
For preparing the raw materials which will be used in the
polymer composite hydrogel some pretreatment steps have
been conducted.
In some cases, there is a process for heating the mono-
mer before staring the reaction, Fig. 15 shows a device for
use in a continuous heating technique to heat an aqueous
solution of an acrylic acid-based monomer [91].

Production Steps of Polymer Composite Reaction Step “Polymerization”

Hydrogel

The production of polymer composite hydrogel is composed A cross-sectional view of a mixer that may be used for a pro-
of five main steps which are summarized as follow. cess in line with the polymer hydrogel preparation is shown
schematically in Fig. 16 [92].

13
 Journal of Polymers and the Environment

Fig. 16  Reactor used for the

hydrogel production [92]

Fig. 17  A shredder mill used for cutting the produced hydrogel [83]

Milling the Produced Hydrogel

After the completion of the hydrogel synthesis, a bulk prod-

uct has been obtained. Before going further, this large piece
should be cut into smaller pieces using a suitable cutting
technique. Figure 17 illustrates a mill used for cutting the
produced hydrogel.
Filtration and Washing
Filtration is the process of removing unreacted monomers
and initiator and crosslinker residues from remaining liquids.
One of the commonly used washing techniques is the
washing with 75% ethanol three times is critical for remov-
ing the remaining unreacted monomers [86].
Drying
The drying step is the final step in hydrogel production. In
terms of drying rate, either a conventional shelf-type drying
or a tower-type (as shown in Fig. 18) drying according to
this invention may be used for the hydrogel drying.
Fig. 18  Tower dryer [93]
Hydrogel Applications
In the following section some of the main hydrogel appli-
cations will be discussed.
Agricultural Applications
The behavior of a slow-releasing hydrogel for ­N H 4+,
­H2PO4−, and K ­ + in soil has been studied [94]. Slow-release
environmental and economic problems are successfully
addressed by polysaccharide-based St, which increases fer-
tilizer consumption efficiency and decreases the frequency
of water irrigation [3].
Additionally, ammonium nitrate (N source) and potas-
sium dihydrogen phosphate (PK source) have been stored
using crosslinked AA/CS hybrids because the latter is dif-
ficult to do so in its natural condition due to its explosive

13
Journal of Polymers and the Environment
Table 5  Application rates of Types of soil
hydrogel in different type of
soils Arid and semi-arid regions
For all level of water stress treatment and improved irrigation period
Sandy soils
To reduce irrigation water by 50% in loamy soil
To improve relative water content and leaf water use efficiency
To reduce drought stress
To prohibit drought stress totally
To decrease water stress
nature. Chitosan was combined with cellulose to reduce the
acid resistance and enhance the mechanical characteristics
[64].
Table  5 shows the various soil types and the recom-
mended appropriate dosage of hydrogel that may be utilized
for them [64].
The application of polymeric composite hydrogel as a
soil conditioner used to improve the aggregate conditions
and also to reduce soil erosion and to prevent crust forma-
tion and general stabilization. The main effect of using
hydrogel in agricultural may be summarized as follows [3].
To test the soil's ability to hold water and its degradabil-
ity, a new superabsorbent based poly (aspartic acid) hydro-
gel has been created. Results showed that after 23 days
of treatment, the maximum water content was 22.6%.
The microbe destroyed 47.8 wt% of the substance [95].
According to Yang et al., double-coated fertilizers could
be created by mixing liquefied corn stover and isocyanate
with biobased polyurethane. Chicken feather protein was
infused into the hydrogel network at the same time. Corn
had a 25.6% better nitrogen-utilization efficiency than
urea-treated corn [96].
Soil Fixation
Hydrogel improves the stabilization and solidification of soil
by varying the physical and chemical features of soil. Hydro-
gel can incorporate to improve water retention in the soil.
Soil Conditioning
Hydrogel aids to increase the available water content of soil
to improve plant growth.
Suggested hydrogel dosage
4–6 g/kg soil
2.25–3 g/kg soil
0.2–0.4 g/kg soil
2–4 g/ plant pit
0.5–2 g/pot
0.2–0.4% of soil
225–300 kg/ha
3% by weight of soil
Soil Erosion Control
Wind and rain are of the most significant environmental
problem for agricultural land. As a method for solving these
problems, hydrogel is applied to aggregate the soil by sur-
face treatment and hence provide surface stabilization during
the early phase of crop growth.
Seepage Control
Hydrogel acts as a membrane in the soil that restricts the
movement of water, thereby protecting crops from salt
damage.
Biomedical Applications
Hydrogels, which have applications in medical implantable
devices, robotic grippers, diagnostic tools for artificial mus-
cles, stabilization of bone implants, intimal thickening in ani-
mals, and reducing thrombosis, mimic the behavior of human
organs in response to changes in environmental conditions
such as pH, temperature, enzymes, and electric fields [19–25,
27–72, 74–98].
Contact Lenses
Hard contact lenses are primarily based on hydrophobic
materials such as PMMA or poly (hexa-fluor isopropyl meth-
acrylate) (HFIM), whereas soft lenses are based on hydrogels.
Soft contact lenses can be produced with different techniques,
such as spin-casting, mold-casting, and lathe-cutting. A poly-
meric hydrogel should have a high oxygen permeability [99].
The equilibrium water content (EWC) of a hydrogel is
defined as:
EWC = m∕mtot × 100%
­ tot is the
where m is the weight of water in polymer and m
total weight of hydrated polymer EWC could change with
13

temperature, pH, and osmolarity. For example, PHEMA
contact lenses contain approximately 38–40% of water in
the fully hydrated state. They typically show low variability
with changes in external factors [99].
Wound Dressing
The primary commercial focus is shifting to the research
and development trend of hydrogels as polymeric temporary
dressing membranes. Thus, certain commercial hydrogels
have entered the market as dressing materials, with brand
names including "Geliperm," "Curasol," and "Tegagel."
By chemically crosslinking acrylamide and methylene-bis-
acrylamide with polysaccharides, these hydrogels were cre-
ated [100].
As damaged tissue is placed and covered by healthy tis-
sue, hydrogel provides a semipermeable surface that allows
normal sodium discharge to occur [101].
The following explanations were used in the initial
attempts by biomaterial scientists to argue that hydrogels as
dressing membranes satisfy all standards for wound healing
and are suitable candidates for burn victims in the quick-
est period possible: (1) Hydrogels regulate the body's lost
liquids and fluid loss; (2) they keep the wound area moist
and wettable; and (3) they have a structure and compatibility
similar to tissue. The benefits listed above apply to most
polymeric dressing materials, such as hydrogels, foams,
films, hydrocolloids, and alginates [102].
Drug Delivery
Before placing the hydrogel-drug complex in the body,
hydrogels are usually formed outside of the body and
impregnated with drugs [103]. Different drugs have been
loaded into the hydrogel backbone. Many factors that are
controlling the release of the medication in a model of the
human body. pH is the most important factor that affects how
drugs are released from hydrogels [23]. Other important fac-
tors include the hydrogel's composition, geometry, manufac-
turing method, type of drug, and environmental conditions
during the release period [104].
For solutions containing 8% by weight or volume of salt,
turbidity variations of chitosan and chitosan/glycerol phos-
phate solutions have been observed over time. At 37 °C, the
turbidity of the chitosan solution did not appreciably alter
over time [22].
Chitosan hydrogels crosslinked with glutaraldehyde had
600–850% swelling values, which reduced when increasing
the glutaraldehyde concentrations. Rapid hydrogel swelling
(less than 20 min, for example) can lengthen the period that
medications remain in the stomach and prevent early gas-
tric emptying [105]. Additionally, the hydrogels' mesh size
13
Journal of Polymers and the Environment
increases throughout the biodegradation process, allowing
pharmaceuticals to diffuse out of the hydrogels [7].
Tissue Engineering
One of the main elements of extracellular matrices is chi-
tosan (ECM). Chitosan is a perfect three-dimensional milieu
used for cell encapsulation because it is biocompatible,
biodegradable, hydrophilic, and non-toxic—features that
are similar to those of the natural ECM. These character-
istics make it a popular choice for a scaffolding material in
cell-delivery treatments and tissue engineering. However,
because chitosan scaffolds lack the mechanical character-
istics of real bone, they are unable to support the weight of
bone implants. Furthermore, chitosan's hydrogels are fre-
quently too soft and delicate to be employed in tissue engi-
neering applications that call for substantial load-bearing
qualities since chitosan itself is not osteoconductive, pre-
venting it from emulating the characteristics of actual bone
[6, 106].
Microneedles (MNs)
As the name suggests, MNs are tiny needles that are often
placed in an array to pierce the protective layer of the skin
and offer a minimally invasive method for the transdermal
delivery of drugs that are typically too large to be absorbed
through the skin. The outermost layer of skin, known as
the Stratum Corneum, is the main barrier to the delivery of
transdermal medications. MNs have the ability to pierce this
barrier, establishing a direct route for the effective adminis-
tration of drugs [19].
Hydrogel-Forming Microneedles (HFMs), the newest
type of MN, were discovered for the first time in 2012. The
other MN kinds previously discussed have a different mecha-
nism of action than HFMs, which are made of crosslinked
hydrogels that can swell. Due to the hydrophilic nature of
the hydrogels, which allows them to readily absorb water,
HFMs will swell when applied to the skin. This makes them
suitable for biological uses such ISF uptake, which is found
around cells in tissue gaps, primarily in the dermis layer
of the skin. ISF can be utilized as a source of biomarkers
as a result, making HFMs a minimally invasive diagnostic
method [103].
MXene Applications
Due to their high surface-area-to-volume ratios, high elec-
trical conductivities (20,000 S c­ m−1), redox capable sur-
face groups, chemical/structural diversities, and large sur-
face-area-to-volume ratios, 2D MXenes with the formula
Mn + 1XnTx offer a large number of promising candidates
Journal of Polymers and the Environment

Table 6  Hydrogels and their biomedical applications

Application Hydrogel Application Refs.

Wound healing Methacrylate, nanofiller enhanced Dressing, cream [108]

Dental Peptide and collagen-based Implant, dressing, cream [58–60]
Drug delivery Stimuli-responsive, nanofiller enhanced, peptide-based, collagen-based, Implant, dressing, contact lenses, [109]
molecularly im- printed polymer (MIP) based soft-gel capsules
Ophthalmic Methacrylate, gelatin Micro emulsion eye drop, con- [110]
tact lenses
Cardiac Nanofiller enhanced, gelatin, stimuli-responsive, self-oscillating Bio-actuator, implant [111]
Organ culture Gelatin, collagen, peptide, stimuli responsive Scaffold [112]
Plastic surgery Hyaluronic acid (HA), stimuli-responsive, meth-acrylate Trans-dermal implant [31]
Cosmetics HA, stimuli responsive, meth- acrylate Cream, dressing [78]

Fig. 19  The way hydrogels act in water purification by contaminant adsorption [114]

for designing conductive 2D hydrogels. To date, a number Separation Technology

of MXene hydrogels have been created through the use
of filtration, metal ions, graphene oxide, or polymers as
crosslinkers, such as polyvinyl alcohol (PVA), polyacryla-
mide, cellulose, chitosan, poly(acrylic acid), and poly(N-iso-
propylacrylamide), with some success. Despite this, MXene
hydrogel research is still in its infancy and faces significant
obstacles [107].
As there are numerous research have been working in
the synthesis and application of hydrogel in the biomedical
applications, in Table 6 some of these hydrogels and their
related biomedical applications have been summarized.
Due to several non-biodegradable, poisonous, and carcino-
genic industrial processes (particularly in the plastic, paper,
cosmetic, and textile sectors), water contamination is a sig-
nificant environmental issue. Adsorption is therefore viewed
as an affordable and efficient way to get rid of these dyes due
to its qualities, such as flexibility in the choice of an appro-
priate sorbent and in the production of effluents that can be
recycled. As a result, there has recently been a noticeable
increase in efforts to develop hydrogels with rapid adsorp-
tion and desorption rates, simple separation, regeneration,
and high adsorption capacities. Figure 19 illustrates how
a hydrogel works as an adsorbent to remove contaminants
from water. Composite polymeric hydrogel networks with

13
 Journal of Polymers and the Environment

Table 7  Performance of some Hydrogel composite HM HG dose g/L Ci (HM) pH qmax mg/g Refs.
composite hydrogel for heavy mg/L
metals removal [73]
Methoxy ethyl acrylamide/clay pb(II) 0.1 100–300 5 81.02 [88]
Polyacrylate-co-PAA/montmorillonite Mn(II) 4 5 275.8 [115]
Cu(II) 5.5 137.3
Zn(II) 5 124.2
St-g-PAA/montmorillonite Cu(II) 4 508 4 102 [116]
Ch/bentonite Cr(VI) 1 100–300 2 89.1 [117]
Sodium polyacrylate/bentonite pb(II) 1 100–300 6 70.5 [118]

Table 8  The different polymer hydrogels for dye removal
Adsorbent Dye Qmax (mg/g) Refs.
Gelatin hydrogel (GH) CV 138.89
MO 72.63
MB 60.328.115
Am-co-AHPS/Oragno-MMT MB 375
N-Tert-butylmaleamic acid MB 405
CV
Xanthan gum-co-AA/GO MB 77.3
Acrylamide-2-methyl-1-propanesulfonic MB 261.78
acid
Wheat straw/Fe3O4 magnetic nanoparti- MB 1374.6
cles
strong water absorption and pollutant immobilization prop-
erties are one of the most promising absorbing materials for
water purification [67]. These composite polymeric hydro-
gels are regarded as advanced composite hydrogels since
they may exhibit various features in terms of gel volume,
swelling, and hydrophilic and hydrophobic surface proper-
ties [113].
Metal ions, which are highly poisonous, non-biodegrad-
able, and carcinogenic, are also regarded as water pollut-
ants, and they have been treated using a variety of thermal,
physical, chemical, electrical, and biological techniques. The
literature has reported on several sorbents made from renew-
able resources. The results of different composite hydrogels
in removing heavy metals are shown in Table 7.
Furthermore, PVA increases the mechanical character-
istics, swelling capacity, and network stability of polymer
hydrogel composite backbones. For instance, the synthe-
sized hydrogel (St/PVA/PAA) adsorbed MB through hydro-
gen bonding and electrostatic interaction. The result was
a higher maximum MB adsorption rate (417 mg ­g−1) than
the CMC/PVA/YE hydrogel [119]. Interestingly, even after
five adsorption–desorption cycles, the St/PVA/PAA hydro-
gel still had a 70% MB removal efficiency, demonstrating
its reusability.
During the pretreat, the St readily binds the hydroxide
ion (OH), increasing its hydrophilicity. Additionally, St's
crystallinity is lost, and the extra ion group that is created is
suitable for higher degrees of graft polymerization, increas-
ing the adsorption capacity [120]. An overview of the out-
[121] comes for dye removal utilizing various polymeric hydrogels
is shown in Table 8.
Given the great diversity among conditions of adsorption
[122] processes in other reported studies, it is difficult to compare
[123] the efficiency of any adsorbent with other adsorbents previ-
ously reported in the literature.
[89]
[113] Biosensor Applications
[124]
Biosensors that detect and convert biological reactions into
a measurable signal have gained much attention in recent
years. A biosensor is a device that uses biological agents
like enzymes and bacteria to detect environmental variables
like pH, temperature, and contaminants like pesticides and
phenols. Biosensors based on acetylcholinesterase as the rec-
ognition component are often utilized for pesticide determi-
nation. Due to their low cost and environmentally favorable
makeup, polymers can also be taken into consideration for
the production of the electrodes for biosensors.
Flexible strain sensors (FSSs) have proven to be a prom-
ising candidate for smart wearable devices due to their
flexibility, light weight, and biocompatibility, as opposed
to traditional devices fabricated from metals or semicon-
ductors, which can only sense small deformations less than
5% strain and are accompanied by inherent rigidity, making
them uncomfortable to wear.
Chaff films and membranes, which are biopolymers, can
be used as surfaces to immobilize biological analytes. Fig-
ure 20 illustrates the benefits of employing chitosan-based
composite hydrogels for biosensor applications [64].
A priority pollutant with the potential to irritate the skin,
eyes, and respiratory system is 4-nitrophenol. The detection
of 4-nitrophenol in water samples has been accomplished
using zinc oxide nanoneedles grafted with CS. With a limit
of 0.23 M, lower concentrations of 4-nitrophenol could be
detected, and the sensor showed a broad linear response
range. It was found that these needles worked well even
when they were near things that could mess with them [64].

13
Journal of Polymers and the Environment
Fig. 20  Advantages of using chitosan for biosensor applications
Oil Recovery
Controlling the amount of water in industrial oils and fuels
is essential for preventing deterioration during storage and
ensuring their intended performance.
Hydrogels are frequently injected near the wellbore to
selectively seal the zones with greater permeability or frac-
tures to reduce surplus water production and hence boost
hydrocarbon production. This directs the injected water
towards low-permeability, upswept hydrocarbon-rich zones
[125].
Polymer hydrogels can be employed as blocking gels to
alter the properties of the rock and the displacement process,
improve sweep efficiency, and ultimately increase oil recov-
ery rates. These systems generally have radial penetration of
5–15 ft (1.5–4.5 m) and are injected into the reservoir forma-
tion via an injection well or a producing well. To seal the
most porous areas, the gel must flow to those areas and build
an impenetrable barrier in the rock's pores. This process can
cause the amount of water to go down and the amount of oil
to go up [22].
The volume to be treated, the kind of base oil, and the
amount of water to be removed all play major roles in deter-
mining which option is the most economically and techni-
cally feasible. For oils with a high-water content, physical
unit operations including gravity separation, centrifuging,
and coalescing filters are often used. However, mass transfer
processes such as distillation and salt beds are frequently
used technologies for processing oils with low water con-
centrations [23].
The water content may go beyond the solubility limit
during the refining, transporting, or storing process, creat-
ing suspended and free water [11]. Water becomes a con-
taminant and causes phase separation when it is suspended
and free. While some suspended waters could naturally split
over time, others might stay suspended forever [15]. The oil
and free water may transfer momentum during the pumping
process, causing temperature changes and the formation of
suspended water, which disperses the water in tiny droplets
[23].
13

Environmental Assessment of Polymer
Hydrogel
Many attempts have been made to construct hydrogel-based
materials for medical and pharmaceutical applications to
minimize the unfavorable systemic toxicity of medicines
and dosage strength. The pharmacies have a wide selection
of hydrogels that have received clinical approval. The pri-
mary need for using a polymeric hydrogel is that it must
be biocompatible with the tissues around it. Materials that
do not include cytotoxic precursors or soaking products are
required for hydrogel systems. The vitality of cells and their
proliferation are important metrics for the biocompatibility
assessment. Only in situ hydrogels are utilized for encapsu-
lating cells [24, 26].
At first, synthetic hydrogels couldn't be used in medicine
because the unreacted monomers and cross-linkers were
toxic, they didn't break down easily, and they couldn't form
hydrogels in physiological conditions [25].
For their use in human applications, hydrogels must first
be created with a low number of leftover reactants and unde-
sired side products. This makes it crucial to rinse them out
of synthetic hydrogels using the proper solvents before ana-
lyzing them. In polymers manufactured for industrial-scale
applications, residual monomer content of up to 0.5 percent
and even up to 1 percent or more is frequently seen [27].
Following the production of the poly (hydroxyethyl meth-
acrylate/methacrylic acid) hydrogel, the remaining reactants
were cleaned with distilled water [28]. The synthesis was
carried out using radical polymerization and ethylene glycol
dimethacrylate (EGDM) as a cross-linker at various concen-
trations [30]. Unreacted monomers and cross-linkers were
removed from synthetic P(AA/methacrylic acid (MAA))
hydrogels with acetonitrile, while Poly(N-isopropylacryla-
mide) (PNIPAM) hydrogels were removed with methanol.
The reactants left behind after the production of P(AA/
MAA) and NIPAM-based hydrogels also demonstrated a
successful polymerization process [28]. Chemical and physi-
cal approaches are used to decrease the residual reactants,
and it was found that the two most popular equipment types
for ensuring the removal of residuals are gas chromatog-
raphy (GC) and high-performance liquid chromatography
(HPLC) [126].
Hydrogel Toxicity
The level of harm that a chemical compound or specific
chemical combination may do to an organism is known as
its toxicity. The negative outcome might range from a small
side effect to a serious threat to the patient's life or survival.
Acute, subphrenic, and chronic toxicity are all possible. A
single or brief encounter can have adverse consequences for
13
Journal of Polymers and the Environment
an organism, which is known as acute toxicity. The capac-
ity of a toxic agent to have effects that last longer than a
year but shorter than the lifetime of the exposed organism is
known as subphrenic toxicity. A substance's capacity to have
negative effects over a lengthy period is known as chronic
toxicity [127].
Low toxicity refers to toxicity that is substantially lower
than acute toxicity, which varies depending on the drug and
the medium's concentration. Toxicology is a dose-dependent
characteristic, and lately, a "Drug Toxicity Index" was estab-
lished, where the author offered mechanistic insights and made
clinical predictions. Effects on the target can be used to gauge
toxicity. Utilizing the median lethal dose (LD50) and the 50%
fatal concentration, the lethal dosage of a toxin, radiation, or
pathogen is calculated (LC50). Furthermore, it has proposed
numerous phrases and the toxicology's lethal dose [96].
Hydrogel Regeneration and Reuse (Recycle)
One of the key components of water treatment technolo-
gies that involves managing its economy is the desorption
and regeneration of adsorbents in the removal of absorbates
(heavy metals, dyes, etc.). Thermal, ultrasonic, chemical,
and electrochemical desorption methods are often utilized.
Electrical enhancement was first introduced fundamentally
and at the adsorption and desorption phases because of the
improvement of chemical desorption procedures through the
use of electricity in various ways [128].
Polyacrylonitrile-based hydrogel has been synthesized
and determined its suitability for electrically assisted regen-
eration in order to increase the effectiveness of heavy metal
adsorption from aqueous solutions in comparison to chemi-
cal regeneration. The results showed that electrically assisted
chemical regeneration had significantly higher nickel and
chromium values of 51.6 and 98.3%, respectively, demon-
strating the benefit of using electrically assisted chemical
regeneration to improve the application of heavy metals-
adsorbing hydrogels [128].
A chelator-mimetic multi-functionalized hydrogel with a
high metal adsorption efficiency (cadmium, lead, and arse-
nic) and great reusability has been synthesized. By using
a low concentration of hydrochloric acid, the heavy met-
als absorbed in the hydrogel network were eluted and the
hydrogel was regenerated for reuse. After five adsorption/
desorption reuse cycles, a removal ratio greater than 60%
was obtained [129]. By applying a similar approach, a novel
hydrogel containing chitosan, acrylic acid has been devel-
oped, and an amine-functionalized nano-silica. In this study,
a 1 molar solution of hydrochloric acid was used to recover
­Pb2+-loaded hydrogel. The hydrogel was then regenerated by
filtering and washing with deionized water before being uti-
lized for the next adsorption cycle. After three consecutive
Journal of Polymers and the Environment
cycles, the efficiency of the regenerated hydrogel remained
around 685–715 mg/g [130].
According to a different study, the determined rates of
photobleaching the dye with the same photocatalyst are 0.02,
0.018, and 0.009 ­min−1 for the first, second, and third experi-
ments, respectively. As a result, the T ­ iO2 supported on the
copolymer hydrogel could be used two to three times [131].
Challenges and Future Development
Activities
The best hydrogel manufacturing and synthesis factories
are those that are small to medium-sized. Therefore, finding
a cross-linking technique that is effective, safe, and envi-
ronmentally friendly is crucial for creating biocompatible
hydrogels with strong mechanical capabilities.
A greater knowledge of the nature of biomaterials and the
principles controlling their growth is possible thanks to the
scientific and technical tools needed for the development of
biomaterials in the long history of human civilization. The
methodology of science and technology plays a significant
role in directing the development of biomaterials from the
viewpoint of the dialectics of nature. Research in science
and technology has been crucial in the creation of bioma-
terials. Finally, the area of biomaterials has been infiltrated
by nanoscience and technology, and people have gradually
come to understand the enormous development potential of
biomaterials, opening many prospects for relevant scien-
tific researchers. The design and preparation of biologically
functional materials has emerged as one of the most signifi-
cant and active areas in the field of life science and medi-
cal research. This area has drawn increasing interest from
interdisciplinary researchers and clinicians due to the ongo-
ing, in-depth development of science and technology. It is
important to not undervalue this tendency in future growth.
Composite hydrogels should consider the following factors:
(1) The design of the reactor and finding a solution for gel
formation with viscosity problems should be studied
as an example. I may suggest "a rotary heated reactor,
a steam heated reactor, a ribbon mixer with a screw
around the axis, a screw mixer with four baffles, and a
double ribbon mixer."
(2) Enhance all mechanical characteristics to fulfil medical
application criteria.
(3) Another important factor to consider for the sporty
treatment of pollutants is short equilibrium times or
fast kinetics.
(4) Make polymer hydrogels biosafe and increase their
effectiveness.
(5) The recovery of hydrogel from solution after the
accomplishment of the adsorption (or desorption) pro-
cedure. (Conventional segregation or
(6) Investigate composite modification using cutting-edge
new natural functional materials hydrogels to improve
performance.
(7) In order to create new hydrogel materials that can be
tailored to the needs of biomedical applications, it is
necessary to combine new techniques, such as rapid
3D printing technology, genetic engineering, and nano-
technology. Clinical applications also call for additional
experimental investigation and testing.
(8) The hydrogel must be physically and chemically stable
during the successive rounds of adsorption–desorption
treatments (regeneration).
(9) The problem of hydrogel disposal should be widely
discussed.
Conclusions
In general, there are many different fields of study that fall
under the umbrella of hydrogel research, and there are an
increasing number of uses for hydrogels. Therefore, it is
challenging to make reliable predictions about the direction
of hydrogel research.
Benefits of Hydrogels that are environmentally sensitive
have the capacity to recognize changes in pH, temperature,
or metabolite concentration and release their load as a result.
Hydrogel is more elastic and durable. Polymeric composite
hydrogels have a variety of special qualities that qualify and
enable them to display amazing properties, allowing them
to be used as viable candidates for applications in nearly all
domains, including biomedical, industrial, environmental,
and agricultural areas. Significant changes are occasion-
ally made to the field of hydrogels for their beneficial uses.
The categorization of polymeric hydrogels and their most
recent developments have been briefly reviewed in the cur-
rent study.
Author Contributions  MME: the only author for this review.
Funding  Open access funding provided by The Science, Technology
& Innovation Funding Authority (STDF) in cooperation with The
Egyptian Knowledge Bank (EKB). The authors have not disclosed
any funding.
Declarations 
Competing interests  The authors declare no competing interests.
Open Access  This article is licensed under a Creative Commons
Attribution 4.0 International License, which permits use, sharing,
13

adaptation, distribution and reproduction in any medium or format,
as long as you give appropriate credit to the original author(s) and the
source, provide a link to the Creative Commons licence, and indicate
if changes were made. The images or other third party material in this
article are included in the article's Creative Commons licence, unless
indicated otherwise in a credit line to the material. If material is not
included in the article's Creative Commons licence and your intended
use is not permitted by statutory regulation or exceeds the permitted
use, you will need to obtain permission directly from the copyright
holder. To view a copy of this licence, visit http://​creat​iveco​mmons.​
org/​licen​ses/​by/4.​0/.
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