Materials Science & Engineering C 114 (2020) 111023

Contents lists available at ScienceDirect

Materials Science & Engineering C

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

Review

Hydrogel membranes: A review T

a b,⁎ a a
Mohsen Khodadadi Yazdi , Vahid Vatanpour , Ali Taghizadeh , Mohsen Taghizadeh ,
Mohammad Reza Ganjalia,c, Muhammad Tajammal Munird,e, Sajjad Habibzadehf,
⁎
Mohammad Reza Saebg, Mehrorang Ghaedih,
a
Center of Excellence in Electrochemistry, School of Chemistry, College of Science, University of Tehran, Tehran, Iran
b
Department of Applied Chemistry, Faculty of Chemistry, Kharazmi University, Iran, Tehran
c
Biosensor Research Center, Endocrinology and Metabolism Molecular-Cellular Sciences Institute, Tehran University of Medical Sciences, Tehran, Iran
d
College of Engineering and Technology, American University of the Middle East, Kuwait
e
Department of Chemical and Materials Engineering, The University of Auckland, New Zealand
f
Department of Chemical Engineering, Amirkabir University of Technology (Tehran Polytechnic), Tehran, Iran
g
Department of Resin and Additives, Institute for Color Science and Technology, P.O. Box: 16765-654, Tehran, Iran
h
Chemistry Department, Yasouj University, Yasouj 75918-74831, Iran

A R T I C LE I N FO A B S T R A C T

Keywords: Hydrogel membranes (HMs) are defined and applied as hydrated porous media constructed of hydrophilic
Membrane polymers for a broad range of applications. Fascinating physiochemical properties, unique porous architecture,
Hydrogels water-swollen features, biocompatibility, and special water content dependent transport phenomena in semi-
Tissue engineering permeable HMs make them appealing constructs for various applications from wastewater treatment to bio-
Separation
medical fields. Water absorption, mechanical properties, and viscoelastic features of three-dimensional (3D) HM
Energy storage
networks evoke the extracellular matrix (ECM). On the other hand, the porous structure with controlled/uniform
pore-size distribution, permeability/selectivity features, and structural/chemical tunability of HMs recall
membrane separation processes such as desalination, wastewater treatment, and gas separation. Furthermore,
supreme physiochemical stability and high ion conductivity make them promising to be utilised in the structure
of accumulators such as batteries and supercapacitors. In this review, after summarising the general concepts
and production processes for HMs, a comprehensive overview of their applications in medicine, environmental
engineering, sensing usage, and energy storage/conservation is well-featured. The present review concludes with
existing restrictions, possible potentials, and future directions of HMs.

1. Introduction
Hydrogels are crosslinked three-dimensional (3D) networks of
highly hydrophilic polymers that can absorb a large amount of water or
biological fluids [1]. A diverse range of hydrogels has been developed
based on natural and synthetic polymers, their derivatives and blends to
fulfil special requirements such as tissue engineering [2], drug delivery
[3], and wastewater treatment [4–6]. The water-swollen hydrogels are
soft materials that can mimic the mechanical properties of animal tis-
sues, highly favorable in regenerative medicine [7]. Furthermore, hy-
drogels have been used in various forms including scaffolds [8,9], in-
jectable hydrogels [10], nanogels (i.e. hydrogel nanoparticles) [11],
microgels and microspheres (e.g. for encapsulation of cells or ther-
apeutic agents) [12], nanofibers [13], and relatively thin films known
as hydrogel membranes (HMs).
On the other hand, membranes are barriers that selectively allow
some moieties to pass through while blocking the others. This process
depends primarily on the pore size and constructing materials of the
membranes [14]. Membranes are widely used in water and wastewater
treatment, gas separation, food and beverage industries, medical and
pharmaceutical applications. Synthetic membranes based on hydro-
phobic polymers and ceramics have commercialised for different ap-
plications, especially water treatment [15]. Polymeric membranes are
usually made of a thin layer of natural derived (e.g. cellulose acetate
and nitrocellulose) or synthetic (e.g. polysulfone, polyethersulfone, and
polytetrafluoroethylene) polymers and may have a porous (in which
separation is based on pore size differences) or dense (in which se-
paration is based on solubility and diffusivity difference of molecules)
structure [14]. Permeability, selectivity, and flux are the most im-
portant characteristics of the membranes. Besides, membrane filtration

⁎
Corresponding authors.
E-mail addresses: vahidvatanpour@khu.ac.ir (V. Vatanpour), m_ghaedi@mail.yu.ac.ir (M. Ghaedi).

https://doi.org/10.1016/j.msec.2020.111023
Received 21 March 2020; Received in revised form 22 April 2020; Accepted 26 April 2020
Available online 30 April 2020
0928-4931/ © 2020 Elsevier B.V. All rights reserved.
M.K. Yazdi, et al. Materials Science & Engineering C 114 (2020) 111023

Nomenclature HRP horseradish peroxidase

iDAA dopamine acrylate
2D two-dimensional IgG immunoglobulin G
3D three-dimensional IPN interpenetrating polymer networks
AA acrylic acid MB methylene blue
AAm monomers acrylamide MBAA N,N′methylenbisacrylamide
AC artificial cell MBGNs mesoporous bioactive glass nanoparticles
AMP ampicillin MIP molecularly imprinted polymer
ASCs adipose stem cells MIT molecular imprinting technology
BBB blood-brain barrier MOFs metal–organic frameworks
BC bacterial cellulose NaCMC sodium carboxymethyl cellulose
BSA bovine serum albumin OOC organ-on-chip
CA cellulose acetate PAAm polyacrylamide
CAn carbonic anhydrase PAO polyamidoxime
CaAlg calcium alginate PBS phosphate-buffered saline
CCG chemically converted graphene PDA polydopamine
ChOx cholesterol oxidase PDADMAC/PAA polydiallyldimethylammonium chloride/poly-
CMC carboxymethylcellulose acrylic acid
CO2 carbon dioxide PDMS polydimethylsiloxane
CS chitosan PEGA polyethylene glycol acrylate
CSs covered stents PEG polyethylene glycol
DABC dialdehyde bacterial cellulose PEGDA polyethylene glycol diacrylate
DCMD direct contact membrane distillation PEGDMA polyethylene glycol dimethacrylate
DEA N,N-diethylacrylamide PMAA polymethacrylic acid
DMA N,N-dimethylacrylamide P(NVP-co-DMDAAC) poly N-vinylpyrrolidone-co-diallyl dimethyl
DN double network ammonium chloride
ECM extracellular matrix PPy polypyrrole
EO engineered osmosis PVA polyvinyl alcohol
EPD electrophoretic deposition PVP polyvinylpyrrolidone
FBR foreign body reaction RAFT reversible addition-fragmentation chain transfer
FTIR Fourier-transform infrared spectroscopy RO reverse osmosis
GelMA gelatin methacryloyl ROS reactive oxygen species
GO graphene oxide SiHPMC silanized hydroxypropyl methylcellulose
GTR guided tissue regeneration SSA ulfosuccinic acid
HAMA hydroxyalkyl (meth)acrylate TGs triglycerides
HEA 2-hydroxyethyl acrylate TDN-HM thermosensitive double network nanocomposite hydrogel
HEMA-EDMA hydroxyethyl methacrylate-ethylene dimethacrylate membrane
poly UF ultrafiltration
HIPEs high internal phase emulsions UHF RFID ultra-high frequency radiofrequency identification
HMs hydrogel membranes w/o water-in-oil
hMSCs human mesenchymal stem cells

is categorised as microfiltration, ultrafiltration (UF), nanofiltration, and
reverse osmosis (RO), depending on the pore size of the membrane
[16].
HMs combine the porous architecture and permeability properties
of the thin membranes with dynamic mechanical properties and water
absorption features of the polymer hydrogels. For example, equilibrium
water absorption of polysulfone is less than 2% while hydrogels can
absorb as high as 90% or more, which significantly affects the porous
structure and permeation features of the HMs. Molecules can diffuse
into the porous structure of 3D hydrogels, similar to the permeation
process in membranes; however, slow mass transfer through bulk hy-
drogels limits permeation unless an external stimulus (e.g. an electric
field in electrophoresis) is applied or if the hydrogel is thin enough
[17]. Besides, the rate of diffusion through hydrogel depends on the size
and hydrophilicity/hydrophobicity of permeating molecules. These
features make hydrogel films promising for manufacturing membranes
for diverse applications [18]. Moreover, thin films hydrogels are pro-
mising for various applications such as antifouling/antimicrobial
coatings, cell culture substrates, and wound dressing applications.
It was revealed that gas permeability is significantly higher when
hydrogel absorbs water to swell. In fact, gas permeation through dif-
ferent hydrogel membranes with diverse water absorption capabilities
exhibited that permeability increase with water uptake tending to level
off at a high swelling degree [19]. However, excessive water uptake
results in mechanical properties to diminish and size-selective separa-
tion to be lost. Accordingly, there is a trade-off between water ab-
sorption and mechanical/separation properties. Absorbed water de-
creases mass transfer resistance via increasing inter-chain distance and
providing interconnected transport passageways [20].
From a bionic perspective, membranes are ubiquitous in many
plants, microorganisms, and even in human/animal bodies. Many
physiological barriers resemble hydrogel membranes; however, they
are much more complex, compared to their synthetic counterparts,
including multilayer structures of various cells, fibre networks, and
biofluids. For example, the intestinal mucus layer, which is produced by
goblet cells, is a protective gel barrier containing glycoproteins that
inhibit gut microbiota from diffusing inward [21]. On the other hand,
the cell membrane may be considered as a hydrogel membrane that has
recently utilised for manufacturing hydrogel scaffolds [22]. The cell
membrane is composed of a phosphate bilayer embedded/decorated
with various proteins that not only separate the intracellular species
from the surrounding microenvironment but also provide various
functions such as cell adhesion to the extracellular matrix (ECM) and
signal transduction through multiple receptors. Cell membranes

2
M.K. Yazdi, et al.
selectively allow some nutrients or biological macromolecules to tra-
verse [23]. However, both passive (e.g. diffusion) and active transport
are observed through the plasma membrane. On the other hand, the
blood-brain barrier (BBB) is a membrane of high-density cells that se-
parate blood from cerebrospinal fluid. The BBB provides selective
transport of particular molecules (e.g. water, amino acids, and glucose)
while preventing the passage of pathogens. Furthermore, lung alveoli
provide blood–air barrier where oxygen and carbon dioxide (CO2) are
exchanged [24]. An epithelial layer or lining is part of the alveolar
membrane (i.e. respiratory membrane) which is mainly responsible for
the exchange of gases. These membrane-like structures are also ob-
served in different parts of animals' bodies responsible for special
functions. On the other hand, multilayer hydrogel membranes in the
exoskeleton of American lobster (containing 90% water), which are
constructed from chitin fibres, effectively dissipate mechanical energy
providing the membrane with high toughness [25].
There are many hydrophilic polymers appropriate for manu-
facturing hydrogels for separation applications. Agarose and poly-
acrylamide based hydrogels have been widely used in the separation of
biological moieties, majorly in electrophoresis [26]. However, they are
not considered as membranes because of their thickness; indeed se-
paration is based on net displacement to relatively long distances. In
contrast, thin hydrogel membranes have been used in bioseparation
[27]. Besides, composite of soft polymeric hydrogels and porous
membranes can be manufactured for diverse applications [18]. Fur-
thermore, polyacrylamide hydrogels can be used for bioseparation
[28]. In this review, various applications of hydrogel membranes are
outlined which include tissue engineering, drug delivery, gas separa-
tion, biosensing, energy, and water treatment.
2. Production processes for hydrogel membranes
Different methods such as sintering, stretching, template leaching,
Fig. 1. Schematic representation of different processes for hydrogel membrane fabrication [43–45].
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Materials Science & Engineering C 114 (2020) 111023
phase inversion, and electrospinning have been used for the prepara-
tion of polymeric membranes (Fig. 1). However, more specific methods
have been used for the manufacturing of hydrogel membranes. The
solution casting is the most frequently used method for the preparation
of hydrogel membranes [29]. In this method, polymers are dissolved in
water followed by drying, crosslinking, and in some cases the removal
of an uncrosslinked polymer. However, this method could be accom-
panied by complementary processes such as freeze-thawing to enhance
miscibility [30,31]. Besides, spin casting is also an important method
for preparing thin films or multilayered HMs [32,33]. Spin casting
provides better control over thin-film membranes.
Electrophoretic deposition (EPD) is a mature and economical
coating procedure to fabricate thin and uniform coatings onto con-
ductive substrates [34]. Using this procedure, an electric field is applied
to a suspension containing charges particle, which as a result drives
particles toward conductive electrodes (i.e. substrate) to create ordered
films, coatings, and membranes [35–37]. Film thickness can be con-
trolled by electric field intensity (i.e. the applied voltage and inter-
electrode spacing) and timespan of the process. The EPD is highly de-
pendent on the zeta potential of suspended particles and their con-
ductivity, the viscosity of the dispersion, and solid per cent in suspen-
sion [38]. The EPD has been utilised for various biomaterials, as well
[39]. For example, chitosan (CS) is water-soluble under mildly acidic
conditions while it precipitates at higher pH values. The dissolved CS in
the CS/silk fibroin dispersion moves to reach around titanium cathode
with higher pH values, resulting in CS deposition to create a thin
composite coating onto titanium implants for enhanced cell affinity
[40]. The EPD method has also been used to fabricate hydrogel mem-
branes based on neat CS and neat silk fibroin for better cell adhesion
and growth in cell delivery applications for tissue engineering usages
[41,42].
Molecular imprinting technology (MIT) is a highly selective method
for recognition and separation [46,47]. This method is an effective
M.K. Yazdi, et al.
strategy for the detection of abundant proteins from blood samples
before analysis [48]. Molecularly imprinted polymers (MIPs) resemble
natural antibodies and can be used to recognise and analyse biofluids
[49]. These polymers have been used to make patterned HMs for special
applications [50]. This biocompatible hydrogel-based system does not
affect protein conformation. For example, albumin imprinted HMs
based on p(HEMA-MAP) can effectively deplete albumin from the blood
[51].
Emulsion templating is a technique for the fabrication of highly
macroporous polymers and inorganic materials [52–54]. In this
method, high internal phase emulsions (HIPEs) act as a template to
produce porous polymer structures. The polyHIPEs (i.e. polymerised
HIPE) primarily indicate the hydrophobic polymer with a porous
structure that is synthesized using free-radical polymerisation in a
continuous phase of a water-in-oil (w/o) emulsion [54]. On the other
hand, inverse w/o emulsions have to be utilised for hydrophilic poly-
mers with open cellular structure and excellent mechanical properties
[55]. Such porous hydrophilic polymers can be considered as HMs. For
example, polymerisation of adequate emulsion templates also used for
preparing HMs [56].
The electrospinning is a versatile method to prepare polymeric fi-
bres of tunable diameter using an electric field. Electrospun fibres have
been utilised in diverse fields such as wound dressings, drug delivery,
and filtration [57]. The method can be used to fabricate fibrous and
porous membranes with controlled 3D structures and definite compo-
sitions [58]. Electrospun nanofibrous membranes based on different
materials (e.g. polymers, ceramics, and carbons) can be used in oil/
water separation [59]. Zang et al. manufactured a nanofibrous HMs
based on core-shell fibres using the uniaxial electrospinning method
[58]. The hydrophilic shell of nanofibers was composed of poly-
methacrylic acid (PMAA) while cellulose acetate (CA) constituted the
core material. The fabricated HM exhibited super hydrophilic char-
acteristics while upon immersion in water the PMAA was hydrated and
showed superoleophobic property [58].
For filtration usage, polymer membranes are required to be thin,
mechanically robust, and can be fabricated in a large scale with a cost-
Fig. 2. Schematic illustration showing the fabrication pathway of B-DN gel membrane. First, 5 mL of Tri-block copolymer was added to the spin plate. Following spin-
coating, the plate was immersed in a water bath to form B gel membrane with weak mechanical properties. Subsequently, to increase its mechanical properties the
plate was immersed in a second monomer solution then exposed to UV irradiation to polymerize the second monomer and form B-DN gel membrane [68].
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Materials Science & Engineering C 114 (2020) 111023
effective and straightforward procedure, which makes it challenging.
The vacuum filtration of aqueous dispersions containing polymer and
chemically converted graphene (CCG) has been proposed as a general
method to make multifunctional polymer HMs [60].
The phase inversion methods are easy, scalable, and low-cost
methods for producing membranes on commercial scales [61]. An HM
based on sodium alginate has been manufactured through a phase se-
paration method [62]. In this method, PVA-SA aqueous solution was
spin-cast followed by ionically crosslinking of SA and finally dissolution
of PVA to yield the SA HMs.
The replica moulding using PDMS moulds was utilised to manu-
facture pH- and temperature-sensitive HMs [63,64]. Compression
moulding has been used to fabricate pH-sensitive HMs based on PVA
and cellulose nanocrystals [65]. Oh et al. used a block copolymer as a
template for the fabrication of semipermeable microcapsules composed
of HMs [66]. Nanoporous HM enveloping the capsule selectively allows
some species to exchange.
3. Engineered and bio-inspired hydrogel membranes
Using double network (DN) hydrogels, containing sacrificial bonds,
high mechanical properties (strength and toughness) which is similar to
cartilage, can be prepared [67]. Using the concept of DN hydrogels, Ye
et al. fabricated thin HMs based on a) different triblock copolymers of
polybutyl methacrylate-b-polymethacrylic acid-b-polybutyl methacry-
late with different degrees of polymerisation, and b) monomers acry-
lamide (AAm), N,N-dimethylacrylamide (DMA), and N,N-diethylacry-
lamide (DEA) (Fig. 2) [68].
On the other hand, HMs can be designed to respond to particular
stimuli such as pH, temperature, ionic strength, and so on. For example,
a pH-responsive hydrogel was fabricated using modified chitosan [69].
Biofilm formation, due to the adsorption of proteins, onto biomaterials
is a severe challenge for implants and scaffolds under the physiological
conditions where biofluid containing proteins and cells. In this regard,
developing surface modification strategies to diminish biofilm forma-
tion is an ongoing research field. Zwitterionic polycarboxybetaine are
M.K. Yazdi, et al. Materials Science & Engineering C 114 (2020) 111023

well-known for their fascinating antifouling properties. They resist because biosynthesis and isolation of aquaporin are expensive. Inter-
against proteins adsorption and cell adhesion such that they could be facial polymerisation can be utilised to fabricate robust aquaporin-
used in different applications especially surface modification [70]. On based membranes [78]. Furthermore, bio-hybrid membrane is a ver-
the other hand, the fabrication of the functional PVA hydrogel mem- satile platform for separation and other applications [79].
brane can be very promising. Surface modification of PVA with zwit-
terionic carboxybetaine methacrylate (pCBMA) via a reversible addi-
4. Hydrogel membranes in tissue engineering
tion-fragmentation chain transfer (RAFT) polymerisation has also been
reported [71]. The pCBMA was grafted onto the PVA surface and endow
Hydrogels are used as scaffold in the tissue engineering (TE), be-
HM with anti-fouling properties while preserving transparency.
cause they are biocompatible 3D polymeric substances which can
Hydrogel membranes based on mTransglutaminase crosslinked ge-
provide mechanical support for the cells in the engineered tissues, can
latin has been manufactured and characterised for dynamic tissue en-
mimic the properties of various tissues, simulate the original extra-
gineering applications [72]. The resulting HM exhibited promising
cellular matrix, and eventually degrade themselves to reconstruct tissue
mechanical properties. High stretchability makes it a right candidate for
or organ. Accordingly, many diverse scaffolding materials have been
organ-on-a-chip applications. A copolymer of polyvinylpyrrolidone
developed to support cell growth in 2D or 3D [80]. Hydrogels with a 3D
(PVP) and hydroxyalkyl (meth)acrylate (HAMA) has been used to fab-
porous structure containing high water content, which can promote
ricate highly hydrophilic HMs with tunable properties [73].
nutrients/water/wastes interchange, are promising for TE applications
Biologically inspired engineering (Bionics) plays a vital role in de-
(Fig. 3) [81,82]. Cells attach to hydrogel ligands via adhesive trans-
veloping modern technologies. In membrane technology and desalina-
membrane proteins integrins (i.e. similar to focal adhesion); besides,
tion, nature inspiration has resulted in the development of aquaporin-
they can regulate their functions and interact with surrounding en-
based membranes for sustainable desalination [74]. Aquaporin in-
vironment and neighboring cells through sending and receiving sig-
dicates that the transport proteins embedded in plasma membranes
nalling proteins (i.e. cytokine, chemokine, growth/death/survival fac-
which selectively and actively transport the number of water molecules
tors) which spread in all directions via mass transfer operations.
significantly compared to conventional membranes [75]. Aquaporin-
Appropriate diffusion of these signalling molecules is critically im-
based membranes can provide high flux, satisfactory stability, and
portant for cell growth and proliferation. These features make HMs
improved salt rejection with low energy consumption [76,77]. The
promising for cell culture and many other applications that are dis-
main disadvantage of aquaporin-based membranes is their higher cost
cussed in this section.

Fig. 3. Illustration of different HM applications in tissue engineering. (a) Depicts cytophilic (cell adhesive) and cytophobic (cell resistant) behaviour of alginate/
chitosan HM with different chitosan deacetylation degree against mouse fibroblast cells. Cytophilic HM had higher surface roughness, so that exhibits better cell
adhesion compared to cytophobic HM [83]. (bI) Shows nine layers of colorless (4 layers) and pink (5 layers) HM composed of short tetramer peptide (Ac-IVKC). (bII
and bIII) Illustrates mechanical stability and topography of as-prepared HM, respectively. (bIV and bV) present high viability of human dermal fibroblasts and mouse
corneal endothelial cells seeded in colorless and pink membranes, respectively [84]. (For interpretation of the references to color in this figure legend, the reader is
referred to the web version of this article.)

5
M.K. Yazdi, et al.
4.1. Cell culture systems
The growth of cells under controlled conditions in an artificial en-
vironment (controlled temperature, pH, humidity, and gases) con-
taining nutrients is known as cell culture. Artificial substrates are es-
sential for most of the cells to grow and proliferate. Modified
polystyrene is a well-known substrate in the in vitro cell culture in-
vestigations for both 2D and 3D culture models [85]. However, the
mechanical properties of the cell environment, which are the substrate
materials, affect the cell functions significantly. In this regard, hydro-
gels that mimic the ECM of the cells can provide a better micro-
environment when culturing and investigating cell behaviour under
certain conditions [86].
Hydrogel membranes based on peptides are natural-inspired mem-
branes. In fact, naturally occurring amino acids are polymerised to yield
peptides possessing high biocompatibility. Ultrashort peptides have
been widely utilised in TE applications. For example, tetramer peptide
has been used to make peptide-based thin HM with the high elastic
modulus (~0.9 MPa) for cell culture and layered biostructures appli-
cation [87]. Silk fibroin is another natural protein which has been
utilised to make degradable HM using the EPD method [42]. The HM
support cell adhesion and growth. Besides, it was proposed as a right
candidate for the encapsulation of proteins and cells and artificial skin.
On the other hand, polysaccharides are the most crucial nature-
based polymers with a wide range of biomedical applications such as
HMs. Transparent HM based on chitosan has been fabricated using the
EPD method. The HM possesses high water absorption capability and
excellent mechanical properties that can support the cell adhesion and
growth for mouse fibroblasts. The pro-inflammatory response, due to
these scaffolds, returned to its normal state after three weeks and no
severe inflammation was observed. The scaffolds were proposed that
can be utilised for cell transplantation and artificial skin [41].
3D cell culture platforms better mimic the microenvironment of
cells. Accordingly, a suspended hydrogel membrane based on photo-
sensitive GelMA was observed that can support seeding of the cell and
encapsulation of them, too [21]. Furthermore, the suspended HMs ex-
hibited higher spreading and proliferation of cells in comparison with
2D unsuspended GelMA platforms. More interestingly 3D printing
technology can be applied to these systems, which make these plat-
forms highly promising for in vitro investigations of cellular interac-
tions and cell fate determination under various conditions.
Gao et al. fabricated thin HMs using a multilayer structure of 2-
methacryloyloxyethyl phosphorylcholine polymer and PVA using a spin
coating method [33]. They optimised the number of layers, spinning
rate, and concentrations of aqueous polymer solutions to encapsulate
cells in every layer. This multilayer structure can be utilised as a 3D
model for in vitro investigations of therapeutic agents. It is crucial to
screen which cells secrete reactive oxygen species (ROS) or H2O2 that
play essential roles in intracellular and extracellular processes. Fur-
thermore, PEG-based hydrogel coating on microcarriers surface can
support the expansion of human mesenchymal stem cells (hMSCs) [88].
Khanmohammadi et al. utilised a microfluidic strategy to fabricate
cell-laden gelatin microparticles [89]. Then, the fabricated micro-
particles were encapsulated within anionic polysaccharide-based HMs
(i.e., modified hyaluronic acid or alginate). Horseradish peroxidase
(HRP) was used as a catalyst to oxidise phenolic moieties on modified
polysaccharides. Improved cell adhesion and proliferation were ob-
served for HA-based HMs indicating their capability in cell culturing
and cell transplantation applications.
4.2. Skin tissue engineering
Skin is a soft tissue that covers the outer surface of vertebrates and
protects the internal tissues/organs from physical/chemical damage
and infections. Besides, it provides a substrate for sensory receptors.
The skin tissue can regenerate itself after minor injury (i.e. wounds),
6
Materials Science & Engineering C 114 (2020) 111023
but in more severe conditions, artificial skin or cell transplantation may
be essential. Skin regeneration may be done using substituents such as
acellular scaffolds, dressings that contain allogeneic skin cells, and
grafts that are used for permanent applications [90]. Nowadays, many
commercialised products based on polymeric biomaterials are available
that are utilised in the wound healing process [91]. Polymer hydrogels
have received particular attention in skin regeneration and wound
management [92,93].
Besides, hydrogel membranes can be used in skin tissue engineering.
Wound management is one of the most frequently used applications for
HMs. For example, a PVA/starch/CS HMs containing ZnO nanoparticles
exhibited antibacterial properties that can be used in topical applica-
tions [30]. Furthermore, HM based on cross-linked low molecular
weight chitosan used for treating bacterial skin infection [94]. The
adhesive HM showed good elastic strength and controlled release of
mupirocin through the rabbit's skin and antibacterial effect, as well.
Montaser et al. fabricated a HM based on chitosan and salicylaldehyde/
TiO2 nanocomposite which exhibit antimicrobial activity [95]. Salicy-
laldehyde molecules were used as a crosslinker for chitosan in which
one aldehyde group is present contrary to conventional dialdehyde
crosslinkers such as glutaraldehyde. Besides, salicylaldehyde benefits in
antifungal activity. TiO2 possesses intrinsic antibacterial properties and
improves the mechanical properties of HM [95].
Hydrogel membranes based on sodium alginate have been used in
wound dressing. Besides, hydroxypropyl methylcellulose (HPMC) or
hydroxypropyl cellulose (HPC) was incorporated to improve mechan-
ical properties [96]. The results showed that hydrated HM transfer
water vapour. Furthermore, a sustained release of gatifloxacin form HM
was observed that was related to both diffusion mass transfer and dis-
solution of the polymer. The composite hydrogel was proposed as a
good candidate for wound dressing materials. Furthermore, wound
dressing HM based on anti-bacterial PVA/Starch was manufactured
with glutaraldehyde as crosslinker and turmeric as an anti-bacterial
compound [97].
Moisture retention is vital in wound healing applications because
water loss results in decrease in temperature [98]. Besides, lower water
vapour transmission (WVT) rates denote the HMs inhibit moisture loss
from the wound microenvironment [97].
Bacterial cellulose (BC), which is also known as microbial cellulose,
is a natural biomaterial that is produced by bacteria. It has been widely
used to manufacture hydrogels and wound dressings. However, BC
suffers from a low degradation rate in the human body [99]. Chemical
modifications, such as partial oxidation, have been considered as a
method to enhance the biodegradability of the BC [100]. On the other
hand, modifications to 2,3 dialdehyde bacterial cellulose (DABC) have
been utilised to fabricate biodegradable HM based on BC [101]. The
obtained HM showed stimulated the proliferation of keratinocyte and
fibroblast compared to non-degradable BC. Besides, ampicillin (AMP)
was loaded in DABC HMs. No immunostimulatory was observed for the
wound dressing made of DABC while it manages to prevent the growth
of Escherichia coli and Staphylococcus aureus.
Viezzer et al. used a hydrogel membrane base on a copolymer based
on chitosan and biodegradable polyurethane as a platform for delivery
of mononuclear bone marrow fraction cells for diabetic foot ulcers
[102]. Utilisation of cell-embedded HM in a diabetic rat model showed
improvement of the wound healing process.
The overexpression and deposition of collagen type I and type III,
which is mediated by IL-1β and TNFα cytokines, results in scar for-
mation [103]. Scar tissue bears not only cosmetic defects but also
prevents appropriate movement of the body and may interfere in body
cooling because of lack of sweat glands [104,105]. In this regard,
various methods have been developed to prevent or remodel scar tissue
[106]. Dampening inflammation (e.g., using anti-inflammatory drugs)
is an effective method to prevent scar formation. Accordingly, humic
acid benefiting from antioxidant and anti-inflammatory properties was
incorporated into alginate-based HM [107]. It was observed that the
M.K. Yazdi, et al. Materials Science & Engineering C 114 (2020) 111023

overexpression of the collagen type I was significantly reduced when
HM is utilised as dressing.
4.3. Bone and dental tissue engineering
Bone is a hard and rigid organ in the vertebrates. Bone tissue that is
also known as osseous tissue provides the bone with high rigidity. This
tissue includes different types of cells, and its ECM contains both or-
ganic (mainly Type I collagen) and inorganic (mainly hydroxyapatite)
components [108]. Despite the fact that bone has a high capability to
regenerate itself after injuries slowly, many scaffolds have been de-
veloped for bone tissue engineering applications to accelerate bone
regeneration (Fig. 4) [109]. Besides, load-bearing implants have been
utilised to aid bone regeneration. In this regard, many materials such as
metal and metal alloys, natural and synthetic polymers, and ceramics,
have been used to fabricate implants for bone and dental tissue en-
gineering [110–112]. Hydrogels have been used for various usage in
bone tissue such as filling the bone gaps [113,114]. For example, a HM
based on photo-cross-linkable GelMA has been used for bone tissue
engineering [115]. The GelMA was reinforced with mesoporous
bioactive glass nanoparticles (MBGNs). The osteogenic differentiation
was significantly enhanced with the aid of HMs. An interpenetrating
polymer networks (IPN) of silanized hydroxypropyl methylcellulose
(SiHPMC) and methacrylated carboxymethyl chitosan (MA-CMCS) for
its degradable backbone to use in IPN. The HM was crosslinked using
the in-situ photochemical crosslinking method during 2 min of irra-
diation for guided tissue regeneration (GTR) in dental applications
[116].
Multilayered HM based on chemically converted graphene (CCG)
has been used as a barrier membrane for guided bone regeneration
[117]. Enhanced osteoinductivity and osteoconductivity along with
improved mineralisation were observed for mature lamellar bone in the
rat model which was attributed to the osteogenic activity of CCG and
multilayer nanostructure of HM (Fig. 4b).
Chang et al. fabricated an antibacterial HM based on gelatin/hya-
luronic acid embedded with hinokitiolto (i.e., a bacteriostat) serve as

Fig. 4. HM application in bone tissue regeneration. (aI) Shows schematic of Periosteum regeneration by GelMA-modified mesoporous bioactive glass nanoparticles
(MBGNs) assembled on GelMA (GelMA-G-MBGNs). (aII) depicts that bone cell regeneration in the composites was higher than pristine GelMA [115]. (bI) presented
CCG-based HM applied for reconstructing of calvarial defect of a rat. (bII) Shows the process of guided bone reconstruction. After 4 (early stage) and 8 weeks (final
stage), new bone cells are appeared in the defected area [117].

7
 Table 1
Applications of HMs for tissue engineering and drug delivery.
Base polymers Additives Application Key findings Ref
M.K. Yazdi, et al.

F127, PEG-DA – Cell culture Formation of membranes in microfluidic channels; a simple one step stamping method [131]
for the in-situ formation of hydrogel membranes.
PVA/starch/CS nZnO Wound dressing Satisfactory dressings especially in early stages; high cell viability for HMs (87%); [30]
increased WVTR with CS loading; good antibacterial activity
SA/HPMC or HPC Gatifloxacin (drug) Drug release wound Enhanced tensile strength and elasticity; enhanced WVTR for hydrated HMs; no [96]
dressing microbial growth; sustained drug release from HPMC or HPC-treated HMs;
PVA-SA Bacteriophages and antibiotics Drug release wound Antibacterial and biocompatible HM; proper burnt wound healing microenvironment [132]
dressing provided by HM; local infection prevention by adsorbed bacteriophages and antibiotics;
optimum properties obtained for 1:2 blended PVA: SA HM; significant bacterial
suppression, wound contraction; inflammation reduction;
PVA/starch Ag NPs Wound dressing Increased swelling and moisture retention capacity with NPs loading; good antibacterial [98]
activity;
PVP Collagenase (debriding agents) Protein release, wound High swelling and high gel fraction for PVP electrospun nanofibers; crosslinking: UV and [133]
dressing Fenton reaction; adjustable collagenase release through electrospinning parameters;
Si-HPMC, MA-CMCS Riboflavin (photoinitiator) Dental tissue Relatively short in situ crosslinking time (120 s); synergistic improvement of Young's [116]
regeneration modulus; biocompatible IPN HMs with barrier effect against human cells in periodontal
defects;
Double network (DN) gels: triblock copolymers, polybutyl methacrylate-b- – Biological applications Tough and self-recoverable thin [68]
polymethacrylic acid-b-polybutyl methacrylate + AAm, DMA, and Biocompatible, and postoperative nonadhesive to neighboring organs
DEA,
PES/PAA TMPTA (crosslinker), methylene Drug release High ion exchange capacity, water absorption, and high drug loading capacity; the high [134]
blue (model drug) impact of crosslinker hydrophilicity on HMs; diffusion-controlled release with pH
sensitivity;
PVA, gelatin Zinc (II)–penicillin complex (drug) Wound skin dressing Anti-microbial activity; [135]
PNIPAAm, HA Ampicillin (drug) Drug delivery pH- and thermo-responsive HMs because of HA and PNIPAAm, respectively; enhance [136]

8
water uptake and flexibility with HA incorporation; drug burst release increase with HA
loading; decreased cell viability with HA lading; good antibacterial activity of neat
PNIPAAm HM which diminishes with the incorporation of HA;
PVA/starch Turmeric (anti-bacterial agent) Wound dressing Good mechanical integrity for wound dressing applications; decreased mechanical [97]
properties with turmeric incorporation; high water absorption (> 100%); high moisture
retention (~91%); low WVTR: 52.85 g/m2h;
Anti-bacterial properties (against gram-positive and gram-negative bacteria)
DABC Ampicillin (drug) Wound dressing Enhanced cell proliferation compared to BC; nanofiber structure; biodegradable HM [101]
showing no immunostimulatory effect; high moisture retention; antibacterial effect
against E. coli and Staphylococcus aureus;
KG, SA Flutamide (drug) Drug delivery Decreased swelling with KG loading; enhanced drug release with SA loading; [137]
CS, gelatin 5-fluorouracil (drug) Drug delivery Biodegradable IPN HM; drug release enhancement with gelatin and drug loading; [138]
prolonged release during 12 h;
XG/GG/HA – Tendon-repair Satisfactory mechanical properties even after water uptake; reduced tendon adhesion [139]
after tendon-repair surgery with efficacy similar to Seprafilm (commercial bioresorbable
adhesion barrier); slower degradation rate compared to Seprafilm resulting in log lasting
barrier effect;
Pectin, PVP Salicylic acid (drug) Drug delivery pH-sensitive drug release and water absorption; increasing tensile strength with PVP [140]
loading;
SA, PVA Prazosin (drug) Drug delivery Thin flexible IPN HM for transdermal delivery of prazosin hydrochloride; crosslinking [141]
density-dependent water vapour permeability and drug release; prolonged drug release
during 24 h compared to neat SA and PVA;
PVA, gelatin Salicylic acid (drug) Drug delivery complete esterification of carboxylic acids in gelatin with hydroxyl groups of PVA; [142]
excellent mechanical properties, hemocompatibility, and water retention capability;
drug diffusion coefficient: 1.32 × 10−5 cm2/s

Where, GelMA: gelatin methacrylate; nZnO: nano Zinc oxide; CS: chitosan; HPMC: hydroxypropyl methylcellulose; HPC: hydroxypropyl cellulose; WVTR: water vapour transmission rate; SA: sodium alginate; Ag NPs:
silver nanoparticles; PVP: polyN-vinyl-2-pyrrolidone; CNC: cellulose nanocrystals; Si-HPMC: silanized hydroxypropyl methylcellulose; MA-CMCS: methacrylated carboxymethyl chitosan; PES: polyethersulfone; PAA:
polyacrylic acid; TMPTA: trimethylolpropane ethoxylate triacrylate; PNIPAAm: polyN-isopropylacrylamide; DABC: dialdehyde bacterial cellulose; BC: bacterial cellulose; HA: hyaluronan; KG: Karaya gum; XG: xanthan
gum; GG: gellan gum.
Materials Science & Engineering C 114 (2020) 111023
M.K. Yazdi, et al. Materials Science & Engineering C 114 (2020) 111023

physical barriers for tooth tissue engineering applications [118]. The
HM prevent bone defect from being filled by connective tissues which
interfere with the bone healing process. Genipin was used to highly
crosslink the HM via an amide bond to provide mechanical integrity.
This biocompatible HM can be used in guided tissue regeneration (GTR)
applications [118].
Langerhans for the treatment of diabetic patients [121]. Encapsulation
of plasmid template and ribosome inside a hydrogel membrane are used
to make an AC [122]. Besides, HM can be used for enzymatic reactions
[123].
4.5. Other applications

4.4. Artificial cells
Artificial cell (AC) indicates engineered particles (e.g. liposomes)
that mimic the function(s) of biological cells. Artificial cells are pri-
marily membranes (biologic or polymeric) that encapsulate biological
components in which metabolism is done. The membrane passively
allows small molecules (nutrients, oxygen, growth factors) to permeate
while blocking large molecules (antibodies and immune cells), resulting
in cell metabolism [119]. The membranes for the fabrication of artifi-
cial cells could be polymers, proteins, lipids, or polymer-lipid com-
plexes. Polymer hydrogels are promising materials for making mem-
branes for ACs [120]. The hydrophilic nature, simple structure,
interconnected porous network, and surface biofunctionalisation pos-
sibility make them closely mimic the biological cell membranes and
recapitulate cell-ECM interactions. Microencapsulation, as the most
used artificial cell, has been used for transplantation of islets of
The determination of protein structure with high resolution is
usually carried out by the crystallisation process with optimised con-
ditions. Homogenous nucleation under controlled conditions simplifies
the crystallisation of biological macromolecules such as proteins. In this
regard, nanostructured HM can be utilised as a support for hetero-
geneous crystallisation. Profio et al. fabricated a series of HMs based on
acrylamide (AA) and polyethylene glycol dimethacrylate (PEGDMA)
with different morphologies for protein crystallisation which showed
better crystallisation behaviour compared to conventional methods
[124].
The incorporation of cellulose into PVA can improve its mechanical
properties. For example, cellulose/PVA HMs in ionic liquid solvent
exhibited enhanced mechanical properties and thermal stability [125].
Furthermore, macroporous semipermeable membranes enclosing living
pancreatic islet cells for diabetic patients [126].
On the other hand, HMs can be utilised as a coating material for

Fig. 5. Various drug release mechanisms from HMs. (i) Presents passive and iontophoretic release of methylene blue as a cationic drug from the membrane with
heterogeneous microenvironment and spheroidal hydrogel particles composed of polyethersulfone/polyacrylic acid. (ii) Illustrates of Piroxicam (a non-steroidal anti-
inflammatory drug) release mechanism from modified cellulose nanofibers by periodate–chlorite oxidation. (For interpretation of the references to color in this figure
legend, the reader is referred to the web version of this article.)

9
M.K. Yazdi, et al.
stents which are used in various applications such as endovascular
aneurysm repair. Covered stents (CSs) are emerging alternatives for
bare stents benefiting from stability, drug-eluting capabilities, and can
prevent intimal hyperplasia [127,128]. For example, mussel inspired
HM have been utilised to fabricate CSs to suppress thrombosis
[129,130]. A semi-IPN on polydopamine (PDA), polyurethane, poly-
acrylamide, poly methyl methacrylate was utilised to coat bare-metal
stents [130]. In this thromboresistant CS, PDA improves polymer-stent
adhesion and enhance cell-materials interactions while other polymers
improve the mechanical properties of the HM. Cell spreading, migra-
tion, and proliferation were improved while platelet aggregation and
activities of smooth muscle cell were suppressed [130].
A brief overview of applications of HMs in tissue engineering and
drug delivery is represented in Table 1.
5. Hydrogel membranes as a carrier
One of the outstanding properties of the HGs is their carrier role.
The effective treatment of wounds is vital to guarantee proper wound
closure and healing with appropriate functional and cosmetic out-
comes. The sufficient strength and water-holding capacity of wound
dressing are important. Hemocompatibility suggested that the hydrogel
could be tried as wound dressing and as an implantable drug delivery
system.
5.1. Drug carrier
Hydrogel membrane based on PVA-gelatin has been manufactured
that possesses excellent mechanical properties and water absorption
capacity. Fourier-transform infrared spectroscopy (FTIR) has confirmed
complete esterification of COOH groups of gelatin. The hemocompat-
ibility of the HM makes it promising for wound dressing and drug de-
livery applications [142]. Another symmetric HM was made of poly-
ethersulfone and polyacrylic acid using photoirradiation and liquid
phase inversion method. Besides, a hydrophilic crosslinker was utilised
[134]. A functional ion exchange capacity, mechanical stability, and
excellent water absorption were observed for the HM. In vitro drug
release with methylene blue as a cationic drug was carried out both in
passive and iontophoretic release modes (Fig. 5). The diffusion-con-
trolled release was observed for passive mode with pH sensitivity while
in the iontophoretic mode linear release kinetics was observed.
Sodium alginate/Karaya gum HM was employed as carrier to uptake
and deliver a non-steroidal antiandrogen drug, flutamide, for prostate
cancer treatment [137]. The HM was crosslinked by glutaraldehyde and
drug was successfully encapsulated in the HM. In vitro investigations in
phosphate-buffered saline (PBS) showed that the drug release rate in-
creases with SA per cent in the HM formulation. A pH-sensitive HM
Fig. 6. Preparation pathway of water-swellable and saline-soluble ZEFM [146].
10
Materials Science & Engineering C 114 (2020) 111023
based on sodium carboxymethyl cellulose (NaCMC) and PVA was uti-
lised for the controlled release of valganciclovir hydrochloride which is
an anti-HIV drug [29]. The HM showed a Fickian release at acidic pH
(pH = 1.2) while a non-Fickian behaviour was observed in physiolo-
gical pH (i.e. pH = 7.4). The in vitro release of anticancer drug, 5-
fluorouracil (5-FU), from an HM based on a biodegradable IPN of ge-
latin and chitosan, confirmed controlled release during 12 h [138].
Proctor et al. used ionic HMs based on polyethylene glycol diacry-
late (PEGDA) and dopamine acrylate (iDAA) as an ionic monomer, in
which dopamine serves as a counterion for anionic acrylate [143]. The
ionic HM enhances the rate of dopamine delivery compared to nonionic
HMs that can be useful for retrodialysis applications such as neurolo-
gical disorders.
Nemr et al. fabricated pH-responsive nanocomposite HMs based on
PVA/PVP/and PVA/PEG containing MWCNTs for drug delivery appli-
cations [144]. It was observed that MWCNTs improve the mechanical
properties of HM; besides, the release of the model drug (salicylic acid)
exhibited a non-Fickian mechanism release that depends on pH, i.e.
drug release is higher at neutral pH in contrast to acidic pH.
Plappert et al. fabricated an anisotropic HM containing open-porous
structure based on cellulose nanofibers as a drug delivery patches for
transdermal administration of piroxicam [145]. The high surface area
of the HM (≤500 m2 g−1) provides sufficient adsorption sites for drug
molecules. Surface charge density and the fraction of carboxylate
functional groups significantly affect the drug loading capacity and
release behaviour from HM.
5.2. Protein and gene carrier
Highly porous HMs based on electrospun nanofibers of PVP were
fabricated and crosslinked with UV irradiation coupled with Fenton
reactions [133]. The release behaviour of a model protein (collagenase)
exhibited that the HM can preserve the enzymatic activity of the protein
and release it for 48 h.
Zein is a naturally derived plant protein that cannot be used as
hydrogel because of its inherent hydrophobicity. However, chemical
modification of this protein can endow its hydrophilicity. After cross-
linking using sodium hexametaphosphate, the modified Zein was elec-
trospun to fabricate fibrous membranes (Fig. 6). It was observed that
both pH and ionic strength can stimulate the obtained HMs [146]. The
HM showed good adsorption and release behaviour for positively-
charged proteins; besides, higher biodegradation rate and satisfactory
cytotoxicity were observed.
Modification of Zein was carried out in controlled temperature
condition using citric acid along with acetic anhydride in an acetic acid
as reaction medium.
Burczak et al. were prepared HG membranes by irradiation and
M.K. Yazdi, et al.
chemical cross-linking of PVA in aqueous solutions. Influences of con-
centration and molecular weight PVA, and irradiation dose, in addition
to cross-linking agent amount on the permeation of albumin, insulin
and immunoglobulin (IgG) through the HMs were investigated. In-
creasing the crosslinked density of PVA HM decreases the water ab-
sorption capacity and diminishes the diffusion coefficients for the tested
bio-macromolecules [147].
6. Hydrogel membranes in organ-on-a-chip devices
Organ-on-chip (OOC) devices are up-and-coming in drug screening
and investigation of cell fate under different conditions because it si-
mulates the physiological conditions of the human body [148]. These
devices present microfluidics, mechanical stretch and other physiolo-
gical stimuli to in vitro models, thus considerably improve their de-
scriptive power. In order to simulate the conditions of some organs,
such as lung, that experience more mechanical stresses, some polymeric
membranes have been incorporated into OOC platforms [149].
In most OOCs, porous polymeric membranes are applied as sub-
strates for cell culture. The polymeric shape, material, and morphology
of these membranes are regularly suboptimal, in spite of their sig-
nificance for attaining perfect cell functionality such as differentiation
and cell–cell interaction. The presently polymers applied for prepara-
tion of these membranes often lack appropriate properties, such as
cytocompatibility and mechanical characteristics matching the tissue to
be grown. Membrane characteristics like as surface roughness and
stiffness could critically affect cells, like as their adherence and growth.
For this purpose, innovative HG membranes have been stated for pre-
paration of porous membranes by appropriate shape, porosity, and
surface morphology matching the necessities of OOCs [150].
It is recommended that initial cell adhesion and spreading are
controlled with substrate surface characteristics, like as roughness and
hydrophilicity, while characteristics like as the stiffness of a cell sub-
strate affect later stages of cell growth [151]. Ye et al. [152] researched
the mechanisms included between stiffness of substrate and differ-
entiation with culturing mesenchymal stem cells (MSCs) on PEG hy-
drogels by changing stiffness. The PEG hydrophilicity hindered ad-
sorption of protein and cell adhesion, therefore cells can only attach to
arginine–glycine–aspartic acid (RGD) peptides bound to the surface.
Stiffer hydrogels stimulated osteogenesis, while softer hydrogels caused
adipogenesis. Stiff hydrogels maybe cause to further focal adhesions
and so higher cell tension, persuading osteogenic differentiation, while
less focal adhesions and fewer cell tension on softer hydrogels stimu-
lated adipogenesis.
Wen et al. [153] cultured adipose stem cells (ASCs) on poly-
acrylamide (PAAm) hydrogels by changing stiffness. Soft hydrogels
addressed cells to adipogenic differentiation, but stiff hydrogels di-
rected to osteogenic differentiation.
Engler et al. [154] differentiated MSCs on collagen I-coated PAAm
substrates and exhibited that the lineage of differentiation depended on
the substrate stiffness. Substrates by a stiffness related to muscle
(8–17 kPa) and brain (0.1–1 kPa) led to myogenic and neurogenic
differentiation, respectively, while stiff collagen I substrates
(25–40 kPa) caused to osteogenic differentiation.
These studies showed potential of HGs membranes in developing
the OOCs.
7. Hydrogel membranes in separation processes
HMs could be used as a filtration membrane in separation of pro-
teins, macromolecules, organic compounds, etc. They have capability to
separate a component from gas phase.
7.1. Biomolecules
Fabrication of ion-exchange membranes by outstanding
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Materials Science & Engineering C 114 (2020) 111023
biomolecules adsorption and purification performance acts a significant
role in the biotechnological fields and biopharmaceutical industry.
Usually, ion-exchange column chromatography has been utilised for the
separation and purification of biomolecules. However, the dis-
advantages of the current ion-exchange columns have restricted their
uses, comprising higher pressure drop persuaded with the compaction
of the chromatographic bed under high flow rate, and slowly adsorbing
and eluting process caused by the longer diffusion path of the ion-ex-
change hydrogel particles [155,156]. Instead, ion-exchange hydrogel
membrane chromatography with porous structure have been estab-
lished to purify biomolecules by numerous advantages like as the short
process time, decreased intra-bed diffusion, relative easy packing, and
scale-up [155–158].
Lv et al. [156] were synthesized in situ cis-butenedioic anhydride
grafted PVA hydrogel nanofibrous membranes (CBA-g-PVA HNFM) by
joining electro-spinning method by the grafting-copolymerization
crosslinking. Taking benefits of the large specific surface area which
could obtain plentiful sites accessible for functional groups and bio-
molecules binding, very tortuous and interconnected porous channel
for biomolecules transfer, and improved mechanical strength, the re-
sultant CBA-g-PVA HNFM showed relatively high binding amount,
quick equilibrium time toward the biomolecule template of lysozyme.
Photopolymerisation was used to prepare HM based on poly(2-hy-
droxyethyl methacrylate-ethylene dimethacrylate) poly(HEMA-EDMA)
that are modified with lectin [157]. The HM exhibited excellent ad-
sorption capability for immunoglobulin G (IgG) which indicates its
ability in antibody separation.
Alele and Ulbricht [158] reported fabrication of a PES UF mem-
brane functionalized by UV-grafted amphoteric polymer hydrogel layer
containing of N-[3-(dimethylamino)propyl]-acrylamide (DMAPAA) and
2-acrylamido-2-methyl-1-propanesulfonic acid for removing proteins of
bovine serum albumin (BSA) and lysozyme. Using continuous diafil-
tration, the hydrogel-functionalized PES membrane removed 82% of
LYS and 74% of BSA by 6 and 10 diavolumes within larger time, i.e. 4.0
and 6.8 h, respectively.
7.2. Gas separation
For example, a HM based on polyvinyl alcohol (PVA) for carbon
dioxide (CO2) separation exhibited high selectivity [159]. In fact, CO2
dissolution in water makes HMs very promising in separation processes.
Because of the solubility of carbon dioxide in water, hydrogel
membranes containing a significant amount of absorbed water, are
good candidates for CO2 separation processes. Hydrogel membranes
with high selectivity toward CO2 were fabricated based on PVA and
embedded polydopamine (PDA) nanoaggregates. It was observed that
PDA significantly improved the mechanical properties of PVA HM, i.e.
70% increase in tensile strength and a 120% increase in the tensile
modulus. It was interpreted that pendant amine groups of PDA can
simplify CO2 molecules transport compared to methane [159].
Different water-swollen HMs based on PVA, chitosan, and carboxyl
methylcellulose (CMC), alginic acid and polyvinylamine were prepared
for CO2 separation [19]. Gas permeation at different pressures was
studied to evaluate the effect of water uptake on the gas permeation
characteristics.
7.3. Oil/water
Zang et al. [58] have studied fabrication and application of an
electrospun core-shell CA/PMAA NHM fibre which is sensitive to pH
stimulus. pH-responsive nanofibrous hydrogel membrane containing
core-shell fibres with the improved antifouling property was fabricated
to separate oil/water under acidic, neutral, and basic conditions [58].
The HM is super hydrophilic and exhibits superoleophobic properties
when immersed in water. The permeating flux is significantly impacted
by fibres morphology and pore size distribution of hydrogels which are
M.K. Yazdi, et al.
influenced by the pH of the environment. The HM possesses high se-
paration efficiency and its flux rate is high too that can be used in
wastewater treatment processes. To prepare the electrospinnable solu-
tion, DMF is utilised to dissolve PMAA powder at the temperature of
85 °C. Meanwhile the dissolving process it can be seen that as the
viscosity reduces, the molecular activity of the PMAA improves. After
electrospinning process of hybrid solution, since DMF tends to vapor-
ized, it carried PMAA macromolecular chains toward the outside wall of
fibres which induced to the synthesis of hydrophilic shell. Slow diffu-
sion rate of CA molecules resulting in the formation of supporting core
(Fig. 7).
8. Hydrogel membranes in water/wastewater treatment
Providing fresh water is a great concern in many parts of the world
because the seawater, which constitutes the protects water resource on
the Earth, is not usable with humans, animals, and even most of the
plants. Accordingly, many desalination technologies such as reverse
osmosis are commercialised in response to the growing demand for
freshwater [160]. On the other hand, industrialisation has aggravated
the water supply concerns because of producing a massive amount of
wastewater that is contaminated by various chemical moieties that can
be harmful to the environment. Thus, many technologies (e.g. mem-
brane systems and adsorbents) have developed for wastewater treat-
ment in industrial and municipal sectors [161,162].
However, many hydrogels may fail to be used in separation pro-
cesses because of relatively low mechanical properties. In this regard,
many HMs are provided with porous support which excels both HM and
the substrate. For example, HM coated hydrophobic support has been
utilised in the desalination process [163]. In this study, an ionic liquid
was incorporated to HM to decrease surface hydrophobicity of the PP
support and reduce the fouling of the membrane.
8.1. Adsorption membranes
Hydrogel membranes can be utilised in adsorption of pollutants or
precious moieties from a liquid such as wastewater. The extraction of
uranium from seawater can significantly affect the nuclear energy
sector because seawater contains a high level of this element. Hydrogel
membranes based on polyamidoxime (PAO) and polyacrylamide ex-
hibit high adsorption capacity for uranium [164]. In this semi-IPN
hydrogel, amidoxime groups of PAOs adsorb uranium efficiently com-
pared to other hydrogel adsorbents. This HM can potentially be applied
Fig. 7. Illustration of uniaxial electrospinning fabrication of a super hydrophilic core-shell HM for oil/water separation. The HM used gravidity for separation of
water molecules from emulsion in the wide range of pH from acidic to alkaline condition [58].
12
Materials Science & Engineering C 114 (2020) 111023
in UF [56].
90
Sr and 137Cs are radionuclides that have high fission yields with
half-lives of around 30 years that may release into the water from nu-
clear power plants [165,166]. These species can cause health problems
such that the treatment of contaminated water is essential [167]. Yoon
et al. used PVA based HMs for filtration removal of strontium ions from
wastewater [168]. They used sulfosuccinic acid as a crosslinking agent
for PVA. High adsorption capacity for Sr2 in a wide range of pH from
acidic to alkaline (pH 2–12) and excellent regeneration capability was
observed for HMs. Liu et al. [3] fabricated a HM based on calcium al-
ginate (CaAlg) coated with iron nanoparticles (Fe NPs, ~5 nm) using a
plant-mediated biosynthesis process to remove Cr(VI) [156]. The high
removal efficiency of 99.5% was obtained for Cr(VI) from contaminated
water. The HM protects Fe NPs against oxidation and extends its life-
time such that ion removal efficiency is preserved efficiently during
frequent cycles. On the other hand, HM shows ion-selective behaviour
such that foreign ions have a minor effect on Cr(VI) removal efficiency
[169].
Adsorption is an effective and low-cost method to remove pollutants
from wastewater [170,171]. In this regard, different materials (e.g.
activated carbon, clays, chitosan, metal–organic frameworks (MOFs))
have been used as adsorbents. These adsorbents are very useful for
heavy metal removal.
Chromium is used in electroplating industries where chromium
ions, especially Cr(VI), presence in wastewater can cause health pro-
blems for humans [172]. Thus removing Cr(VI) from wastewater must
be strictly controlled. Accordingly, adsorption of Cr(VI) using different
nanomaterials such as iron nanoparticles have gained much interest.
HMs based on alginate and coated with iron nanoparticles (FeNPs)
showed high capability in removing chromium ion from wastewater
[169].
Ion exchange HM based on cross-linked AMPS/PEGDA was used for
the sorption of water and ions [173]. HMs have been used as catalytic
reactors in which water contaminants are oxidised. Catalyst nano-
particles (Palladium) were embedded in an alginate HM that surrounds
a gas permeable hollow-fibre membrane. During the process, hydrogen
flows into the hollow-fibres where it can partially diffuse into the HM.
Hydrogen molecules (H2) reduce O2 and NO2 contaminants that dif-
fused from bulk aqueous solution into HM [174].
Antifouling HMs based on copolymers of PEGDA and one of acrylic
acid (AA), 2-hydroxyethyl acrylate (HEA), or polyethylene glycol ac-
rylate (PEGA) as comonomers were utilised in oily wastewater treat-
ment [175]. PEGDA acts as comonomers and crosslinker agent. Water
M.K. Yazdi, et al. Materials Science & Engineering C 114 (2020) 111023

absorption and permeability are greatly impacted by crosslink density
and polymer composition such that permeability coefficients for water
were calculated to be 10 to 26 L mm/(m2 h bar). In comparison, the
diffusion coefficients for sodium chloride are nearly independent of the
polymer composition. Furthermore, the fabricated HMs exhibited high
fouling resistance properties which make them promising in wastewater
treatment containing oil residue.
Graphene oxide (GO) is highly hydrophilic nanomaterial because of
various oxygenated groups that are present on this nanoplatelet [176].
Accordingly, itcan absorb high amount of water and can be utilised for
making 3D hydrogels. Chen et al. fabricated HMs based on GO using the
vacuum filtration method [177]. They used ferrous ions (Fe2+) as a
crosslinking agent for GO; high stability, enhanced adsorption capacity,
and increased water permeability were observed for the HMs. The HM
can effectively separate methylene blue (MB) and other organic con-
taminants from water over a wide pH range [177].
Engineered osmosis (EO) membranes utilize the natural phenom-
enon of osmosis for separation applications. Qin et al. deposited a
skinny and smooth layer of HM as the selective layer onto a porous
support layer to improve the performance of EO membrane, as illu-
strated in Fig. 8 [178]. PES/GO nanocomposite constitutes the porous
support layer; a stainless steel knife applicator was utilised to apply
PES/GO/DMF solution on a clean glass plate . PVA aqueous solutions of
various concentrations (i.e., from 0.05 to 1 wt%) were utilised to make
selective layers. In this regard, the support layer was dip-coated in
previously crosslinked PVA aqueous solution for 20 min to deposit HM
selective layer. It was observed that water permeability increases with
the thickness of HM such that a 10-fold enhancement was measured
when the thickness decreased from 500 nm to 30 nm. Maximum se-
paration efficiency was observed for 45 nm-thick HMs (Table 2).
9. Hydrogel membranes in sensors & actuators
Sensors are devices that can provide information about the presence
and amount of chemical species in a fluid phase. Electrochemical sen-
sors for the detection of air pollutants from industrial chimneys and
blood glucose meters are popular sensors for industrial and household
applications. Biosensors are sensors in which a biological component is
used as the recognition element [183]. Electrochemical biosensors are
very promising in the detection of various materials. In this regard,
electrochemical sensors based on protein imprinted material have
gained attention [184]. On the other hand, a molecularly imprinted
polymer (MIP) hydrogel membrane was designed for the detection of
BSA protein [50]. The BSA was incorporated into a sodium alginate
solution and changed into a film using a glass rod twined copper wire.
The film was then ionically crosslinked by calcium ions to yield the HM.
Tris-HCl buffer solution was utilised to remove BSA to produce the final
MIP HMs. In fact, the low thickness of HMs allows sufficient depletion
of BSA through mass diffusion mechanism. The imprinted HM was
loaded on an electrode and the voltammetry curve was utilised to study
the adsorption of BSA. The results exhibited that the BSA rebinding rate
on the imprinted HMs was much faster compared to calcium alginate
microspheres.
A cholesterol biosensor was manufactured using cholesterol oxidase
(ChOx) enzyme embedded in a composite HM based on p(HEMA) and
polypyrrole (PPy) [185]. The biosensor showed a good correlation for

Fig. 8. Structural features and schematic representation of HM production process. (a) AFM and FESEM images determine morphological specifications of HM as the
selective layer. Dome-shaped nanostructures on the top selective layer in AFM images. (b) AFM and FESEM images of the top surface of the support layer. A concave
area in AFM image represented as a green loop. (c) The cross-sectional architecture of the membrane illustrated by FESEM images of different magnification. (For
interpretation of the references to color in this figure legend, the reader is referred to the web version of this article.)

13
 M.K. Yazdi, et al.

Table 2
Applications of HMs for separation processes in water/wastewater industry.
Base polymers Additives Application Key findings Ref

PolyMAA Poly(EHA-co-St-co-DVB) UF applications pH dependency of permeability and rejection of PEG/water solutions; [56]
polyHIPEs
CA, PMAA – Oil/water separation pH-responsive and transparent nanofibrous HM via uniaxial electrospinning; superhydrophilic properties of as-prepared HMs [58]
versus superoleophobic properties of immersed HMs; effective separation under various pH values using gravity force only; pH-
dependent nanofibers micromorphology and pore size, resulting in permeating flux alternation while preserving separation
performance; high separation efficiency and recyclability;
PVA PDA nanoaggregates CO2 separation High mechanical properties of swollen HMs because of PDA (hydrogen bonding) compared to neat PVA; enhanced CO2/CH4 [159]
selectivity (hindering larger molecules) compared to neat PVA; enhanced CO2 permeation because of abundant NH2 groups on
PDA.
PVA Sulfosuccinate acid (crosslinker) Water treatment Excellent mechanical strength; high adsorption capacity for Sr2+ in pH 2–12; excellent recyclability; [168]
SA Pd NPs (catalyst) Water treatment Hydrogenation of contaminant species (O2 and NO2−) through the diffusion of H2; HMs' thickness dependency of reaction rate; Pd [174]
concentration-dependency of byproduct selectivity;
PEGA or AA or HEA PEGDA (crosslinker) Oily wastewater treatment Significant effect of crosslink density on water uptake and permeability; decreased water uptake with increasing PEGDA; higher [175]

14
water permeability with swelling ratio; little dependency of NaCl diffusion coefficients on HM's composition; the low affinity of oil
for HMs resulting in fouling resistance
PVA on PES Graphene oxide Engineered osmosis membranes Water permeability increased; 10-fold enhancement in flux was measured when the thickness decreased from 500 nm to 30 nm. [178]
Maximum separation efficiency was observed for 45 nm-thick HMs.
Natrix – Membrane chromatography High binding capacities for mAbs; high purification efficacy; high loading capacity and high operational speed; comparable pilot [179]
scale and lab-scale results; potential alternative for protein A chromatography;
PVSA MBAA (crosslinker) Ethanol dehydration Polyelectrolyte HMs serves as an active layer (100–300 nm) on PES ultrafiltration support; increased IEC with MBAA up to 5%; [180]
extremely high pervaporation separation index; stability issues;
Kevlar hydrogel Hydrogel/PA thin layer Nanofiltration Hydrogel assisted interfacial polymerisation is reported; high permeances of 62.9 L m−2 h−1 bar−1 while maintaining [181]
satisfactorily high rejections of 96.4% and 93.5% for Na2SO4,
CS Goethite nanoparticles Removal of Congo red dye from Important role of goethite nanoparticles in formatting multi-membranes of hydrogel capsules; [182]
water

Where, PVA: polyvinyl alcohol; CS: chitosan; CMC: carboxyl methylcellulose; ALA: alginic acid; PVAm: polyvinylamine; PEGA: polyethylene glycol acrylate; AA: acrylic acid; HEA: 2-hydroxyethyl acrylate; PEGDA:
polyethylene glycol diacrylate; Natrix: polyacrylate hydrogel with high density of carboxylate groups; mAbs: monoclonal antibodies; PVSA polyvinylsulfonic acid; MBAA: N,N′-methylenbisacrylamide; PES: poly-
ethersulfone; IEC: ion exchange capacity; CA: cellulose acetate; MAA: polymethylacrylic acid; EHA: ethylhexyl acrylate; St: styrene; DVB: divinylbenzene; HIPEs: high internal phase emulsions; PDA: polydopamine; SA:
sodium alginate; Pd NPs: palladium nanoparticles.
Materials Science & Engineering C 114 (2020) 111023
M.K. Yazdi, et al.
cholesterol in serum samples of patients.
Carboxymethylcellulose (CMC) is a water-soluble derivative of cel-
lulose which can be used as sensing material in humidity sensors.
However, water solubility adversely affects the durability of such sen-
sors such that cross-linking should be considered. CMC-based HM
crosslinked by epichlorohydrin acts as an absorbing layer in a resistive-
based humidity sensor [186].
An interesting smart wound dressing was fabricated based on HMs
which has integrated both dressing and monitoring functions [187].
The HM was based on xyloglucan-PVA HM equipped with an ultra-high
frequency radiofrequency identification (UHF RFID) sensor. The HM
can effectively absorb simulated body fluids in the damaged areas and
simultaneously monitored moisture levels in the skin-dressing contact
area (Fig. 9). According to SEM images (Fig. 9a and a′) of as-prepared
HM the surface and cross-section of the HM exhibit homogenously
distributed pores, still heterogeneous in size. Fig. 9b shows SEM image
of HM after immersing in the water for 24 h. The larger pore size
confirmed the swelling of the HM.
Bhat et al. made HMs based on Poly(2-hydroxyethyl methacrylate)
that can potentially be used in biosensors [188]. A HM based on silk
protein was utilised to fabricate water sensors with high sensitivity
[189]. The silk protein swells in the presence of water such that it is
possible to detect water impurities in organic solvents even when H2O
content is as low as 0.008%.
A pectin-based HM was utilised to fabricate an optical biosensor for
the detection of triglycerides (TGs) [190]. The biocompatible HM
serves as immobilising matrix for lipase enzymes while allowing ef-
fective permeability of various analytes in contrast to many im-
mobilising matrix based on synthetic polymers. The immobilised lipase
catalyse TG hydrolysis reaction to fatty acids and glycerol which result
in reduction in pH of the surrounding microenvironment followed by a
color change in a pH indicator. The color change can be detected using
UV–Vis spectrophotometer [190].
Fig. 9. HM for wireless smart wound healing. SEM images of xyloglucan-PVA HM before immersion in a water bath (a and a′), after immersion in the water bath for
24 h (b), and after immersion in saline solution for 24 h (C). Remote monitoring of the healing process by the prepared HM [187].
15
Materials Science & Engineering C 114 (2020) 111023
10. Hydrogel membranes in energy storage and conversion
Storing electrical energy is one of the most important issues for new
technologies such as portable electronic devices and electric vehicles.
Batteries and supercapacitors are the most well-known and widely used
devices for electrochemical energy storage such that it is anticipated to
the electrochemical capacitor market reaches $11 billion by 2022
[191]. Batteries can store much more energy compared to super-
capacitors which are known as energy density while the power density
(the energy release per second) is higher for supercapacitors. A com-
bination of these devices is required in EV applications. Fuel cells, si-
milar to batteries, convert the chemical energy into electrical energy
but in a different way [192].
Polymer membranes have been widely used as a separator in dif-
ferent types of rechargeable batteries and fuel cells. For example,
Nafion membranes are the most popular cation exchange membranes
that are used as a separator for fuel cells [193]. However, the polymer is
high cost such that manufacturing separator based on other polymers
and polymer hydrogel have been grabbed much attention [194]. For
example, HM based on chitosan has been used as a separator for making
rechargeable Al-air coin cells, as shown in Fig. 10 [195]. According to
Fig. 10 chitosan was dissolved in the acetic acid due tom protonation of
the existing amino groups in its structure. After evaporation of acid
molecules in drying process and deprotonation of amino groups, the
membrane was fabricated.
Furthermore, the HM was modified with oxide fillers (i.e. SiO2,
SnO2, and ZnO) to improve the cell performance.
A high performance, flexible electrochemical supercapacitor was
fabricated using SWCNT as electrode and PVA HM as the separator
[191]. The thin HM was soaked in a diluted sulfuric acid solution
(electrolyte) after drying. The obtained capacitor showed a time con-
stant of 15 ms, very high durability after high repeated cycles, and high-
energy efficiencies.
A cationic polyelectrolyte HM based on poly N-vinylpyrrolidone-co-
M.K. Yazdi, et al. Materials Science & Engineering C 114 (2020) 111023

Fig. 10. Schematic illustration of chitosan-based HMs modified with different metal oxides (SiO2, SnO2, and ZnO) [195].

diallyl dimethyl ammonium chloride (P(NVP-co-DMDAAC)) and PVA content in the HM coated ZIF-8/CAn was extremely higher than free
was prepared for solid-state supercapacitors [196]. Higher permittivity CAn and even higher than ZIF-8/CAn, which indicates the importance
(27.19 at 1 kHz) and good ionic conductivity (0.0366 S·cm−1) was of HM in protecting the enzyme [201].
observed for the obtained IPN HM containing 10 wt% PVA, compared Ardeshiri et al. fabricated a semi-IPN HM based on poly-
to PVA or P(NVP-co-DMDAAC). A high retention rate of 95% was diallyldimethylammonium chloride/polyacrylic acid (PDADMAC/PAA)
reached after 1000 cycles; besides, it was observed that specific capa- on PVDF membrane support which shows anti-wetting properties for
citances of supercapacitor decrease with the thickness of HM [196]. direct contact membrane distillation (DCMD) applications [202]
HMs can be utilised to make separators for flexible batteries. (Table 3).
However, most of the HMs (e.g., PEG and PAM) are degradable under
alkaline conditions [197]. However, Huang et al. utilised sodium 12. Conclusions
polyacrylate-based HM as a separator for making flexible hybrid Zn air
metal batteries (ZAMB) [198]. This HM endows batteries with im- Hydrogel membranes are interesting porous structures composed of
proved cycling stability, flexibility, and enhances specific capacity. hydrophilic polymers. The water-rich and porous features of these
constructs have attracted many researchers from interdisciplinary fields
to create novel and robust membranes. The current review paper is an
11. Other applications
attempt to better understand the preparation and characterization of
hydrogel-membrane conjugation which leads to a myriad of applica-
Thin-film Polyelectrolyte HMs have been used to prepare for
tions in diverse fields ranging from biomedical and purification to en-
ethanol dehydration [180]. Poly (vinyl sulfonic acid) crosslinked by
ergy storage and conversion field. In this study, various routes to fab-
N,N′methylenbisacrylamide (MBAA) was used as an active layer which
ricate these membrane types were introduced, with the solution casting
was polymerised onto polyethersulfone support by the aid of UV irra-
approach as the most common approach. The imparting of non-toxic,
diation.
low cost, and affordable hydrogel into the structure of fabricated
Inspired by bioelectrogenic processes, manufactured nanofluidic
membranes for medical application is an ever-growing approach be-
generators use graphene HMs with layered structure [199]. The 2D
cause of the new features that hydrogels could give them, especially
nanogenerator can produce ionic current signals upon exposure to ex-
higher bioactivity, excellent adhesion, and tissue-like mechanical
ternal mechanical forces.
strength. Moreover, the strategy of promoting separating characteristics
Thermosensitive double network nanocomposite hydrogel mem-
of the membranes using hydrogel ingredients made them more favor-
brane (TDN-HM) was used to reduce foreign body reaction (FBR) of
able for environmental applications especially for wastewater treatment
implanted glucose biosensor [200]. TDN-HM constructed based on
and air purification. Intriguing properties such as high porosity along
polysiloxane nanoparticles embedded in PNIPAAm. This thermo-
with controlled pore size and the unique functional group in which
sensitive HM serves as a self-cleaning housing for subcutaneously im-
hydrogel provides membrane enhanced separating capability of them
planted glucose biosensors where it inhibits cellular adhesion and
toward filtration of higher amounts of contaminants, pharmaceutical
biofouling such that long-term functionality of biosensors is guaranteed
agents, or gas molecules adsorption for separation purpose, biomedical
[200].
demands, and energy storage.
Ren et al. used PVA/CS HM as a coating for ZIF-8 for CO2 seques-
tration applications [201]. Carbonic anhydrase (CAn), which can re-
versibly convert carbon dioxide into bicarbonate, was encapsulated into Declaration of competing interest
the metal-organic framework (MOF) structure to enhance its stability.
Excellent CO2 capture performance was observed; calcium carbonate The authors declare that they have no known competing financial

16
M.K. Yazdi, et al. Materials Science & Engineering C 114 (2020) 111023

Where, BSA: bovine serum albumin; SA: sodium alginate; XyG: xyloglucan; SBF: simulated body fluids; PHEMA: poly2-hydroxyethyl methacrylate; PPy: polypyrrole; GOx: cholesterol oxidase; CMC: carboxymethyl
interests or personal relationships that could have appeared to influ-

[185]

[186]
[187]

[191]

[195]

[203]
[50]
Ref
ence the work reported in this paper.

Absorbing layer in resistive-based humidity sensor; good humidity sensing properties in relative humidity ranging from 53 to 93%.

Ion-conducting PVA-based HM (00 μm) for supercapacitors; high ionic conductivity: 10−2 S/cm; thinner hydrogel membranes result

Radio-frequency identification (RFID) integrated into HM; serving as epidermal-tag monitoring wound conditions; absorbing wound
Separator for recyclable Al-air coin cell-type batteries; improved discharge performance, longer discharge, enhanced power density,
HM containing GOx serve as amperometric cholesterol biosensor; linear response range: 5 × 10−4–1.5 × 10−2 M; detection limit:

capabilities of HMs; absorbing a high amount of SBF resulting in swelling and ion mobility alternation followed by electromagnetic
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