Advances in Colloid and Interface Science 305 (2022) 102705

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Advances in Colloid and Interface Science

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

Historical perspective

Nanomaterial based PVA nanocomposite hydrogels for biomedical sensing:

Advances toward designing the ideal flexible/wearable nanoprobes
Zahra Karimzadeh a, b, Mansour Mahmoudpour a, b, Elaheh Rahimpour a, c, *,
Abolghasem Jouyban a, d
a
Pharmaceutical Analysis Research Center, Tabriz University of Medical Sciences, Tabriz, Iran
b
Student Research Committee, Faculty of Pharmacy, Tabriz University of Medical Sciences, Tabriz, Iran
c
Infectious and Tropical Diseases Research Center, Tabriz University of Medical Sciences, Tabriz, Iran
d
Faculty of Pharmacy, Near East University, PO BOX: 99138 Nicosia, North Cyprus, Mersin 10, Turkey

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

Keywords: In today’s world, the progress of wearable tools has gained increasing momentum. Notably, the demand for
PVA hydrogels stretchable strain sensors has considerably increased owing to various potential and emerging applications like
Nanoparticles human motion monitoring, soft robotics, prosthetics, and electronic skin. Hydrogels possess excellent biocom­
Nanocomposite hydrogels
patibility, flexibility, and stretchability that render them ideal candidates for flexible/wearable substrates.
Flexible sensors
Strain sensors
Among them, enormous efforts were focused on the progress of polyvinyl alcohol (PVA) hydrogels to realize
multifunctional wearable sensing through using additives/nanofillers/functional groups to modify the hydrogel
network. Herein, this review offers an up-to-date and comprehensive summary of the research progress of PVA
hydrogel-based wearable sensors in view of their properties, strain sensory efficiency, and potential applications,
followed by specifically highlighting their probes using metallic/non-metallic, liquid metal (LM), 2D materials,
bio-nanomaterials, and polymer nanofillers. Indeed, flexible electrodes and strain/pressure sensing performance
of designed PVA hydrogels for their effective sensing are described. The representative cases are carefully
selected and discussed regarding the construction, merits and demerits, respectively. Finally, the necessity and
requirements for future advances of conductive and stretchable hydrogels engaged in the wearable strain sensors
are also presented, followed by opportunities and challenges.

1. Introduction nanomaterials with stability, biocompatibility, and superb mechanical

Nowadays, highly flexible soft electronics nanoprobes that can
monitor health motions and conditions have attracted considerable
attention for potential applications in soft robotics and wearable tools
due to their comfort and convenient utilization [1,2]. Indeed, these
sensors have capable of converting external stimuli like pressure and
tensile to electrical signals such as voltage, capacitance, current, and
resistance [3,4]. Skin-like wearable sensors are usually assembled from
elastomers and conductive nanomaterials such as inorganic conductive
particles, metal nanowires (NWs), carbon nanotubes (CNTs), and gra­
phene, however, uniformly dispersion of fillers in the elastomer is
problematic. As well, friction could occur between the conductive filler
and the elastomer bringing on stress concentration, which significantly
damages the mechanical property of the probe [5]. Therefore, intro­
ducing intrinsically conductive and flexible polymer-conductive
properties has attracted people’s attention [6,7]. In this regard,
hydrogel-based flexible/wearable nanoprobes different from the rigid
elastomer-based probes exhibit great potential in the sensory field by
easily tuning the mechanical properties, network structure, and chem­
istry of the water-containing hydrogels to match those of bio-tissues,
laying the foundation of designing of smart skins and implantable de­
vices [8,9]. In addition, hydrogels are also one of the most reliable
materials for other applications e.g. wound dressing, tissue engineering,
drug delivery, water treatment [10,11], separation filter [12] rather
than sensing [13] due to abundant hydrophilic intermolecular space for
the entrance of other materials [14].
PVA hydrogel is a synthetic polymer that has sparked great interest
in biomedical fields regarding its advantages such as biocompatibility,
nontoxicity, biodegradability, hydrophilicity, and chemical stability.
Significantly, the myriad of -OH groups on PVA could result in the

* Corresponding author at: Pharmaceutical Analysis Research Center, Tabriz University of Medical Sciences, Tabriz, Iran.
E-mail address: rahimpour_e@yahoo.com (E. Rahimpour).

https://doi.org/10.1016/j.cis.2022.102705
Received in revised form 20 April 2022;
Available online 18 May 2022
0001-8686/© 2022 Elsevier B.V. All rights reserved.
Z. Karimzadeh et al.
development of physical/chemical cross-linked PVA hydrogels in
diverse fields [15–18]. There are many weak non-covalent bonds such as
van der Waals and hydrogen bonding between molecular chains of PVA
in physical entanglement [19]; meantime, there is a chemical interac­
tion between -OH groups on PVA and active moieties in chemical cross-
linkers. The chemical cross-linkers included in the fabrication of PVA
hydrogels could be glutaraldehyde, acetaldehyde, formaldehyde, and
other mono-aldehydes [20]. Physical/chemical cross-linking evolution
of PVA hydrogels in most cases brings about some issues like a lack of
elastic modulus, tensile strength, toughness, and high water loss rate
which should be extensively investigated. Similarly, pure PVA nanofiber
membrane has poor mechanical strength which leads to an easy
reduction in the filtration performance. Currently, hydrogen bond cross-
linking approaches catch the spotlight as they considerably enhance the
mechanical properties of PVA materials with no destruction of its flex­
ibility [21]. The formation of firm inter- and intra-molecular H-bonds
interaction by adding fillers into the spinning solution can increase the
strength [22,23]. In pursuit of improving their performance, new vari­
eties of hydrogels including double network hydrogels [24,25] and
nanocomposite hydrogels [26,27] have been developed. Amongst,
nanocomposite hydrogel has aroused much scientific interest owing to
its improved structural properties and expanded the applicability of
these heterogeneous materials by amalgamating the properties of nano-
sized fillers with hydrogels. Hydrogel matrix can provide not only a host
network for nanoparticles (NPs) as guest nanomaterials; but also act as
nano-reactors for their synthesis due to their inert and semi-wet struc­
tures [28]. Moreover, nanomaterials can donate to the stabilization and
formation of hydrogels, probably functioning as cross-linkers of polymer
chains to reinforce hydrogels [29,30]. Therefore, the incorporation of
nanomaterials into hydrogel matrices results in the formation of PVA
nanocomposite hydrogels with enhanced practically important me­
chanical, catalytic activity, electrical conductivity (by transmitting
either electrons or ions), optical, thermal [31,32], and magnetic prop­
erties [26]. Valuably, these customized functionalities can be adjustably
switched ON-OFF via exterior signals which control the sol-gel transition
of PVA hydrogels [33]. Moreover, it has been reported that sensing
performance and mechanical properties can be tuned by varying the NPs
concentration in the sensing layer and the concentration of PVA in the
supporting substrate [34]. A wide range of NPs introduced into the PVA
polymeric network can be represented by various materials containing
non-metallic, metallic/metal oxide NPs (MONPs) [28], polymeric
[35,36], and bio-nanomaterials having diverse sizes and shapes.
Depending on the type of nano-sized species and polymeric matrix,
nano-species could be embedded into a PVA polymeric hydrogel via
different experimental mechanisms. Growing nano-species inside
hydrogel matrices from a seed-precursor is one of the approaches for the
formation of PVA nanocomposite hydrogel. Another is hydrogel for­
mation in the existence of nanomaterial. Nanomaterial absorption by
pre-formed hydrogels is lastly the other mechanism of NPs entrapment.
These ex-situ or in-situ incorporations can be physical or chemical cross-
linking. The unique characteristics of PVA nanocomposite hydrogel
have revealed high importance for broad variety of biomedical appli­
cations and strain/pressure sensors [37].
Currently, searching for high-performance and ideal nanofillers and
scheming well-defined structures of hydrogel networks are similarly
essential for the practical design of PVA nanocomposite hydrogel-based
wearable sensors. Meanwhile, the feasible and facile combination of
hydrogels and nanofillers without destructing other features is still ur­
gently desired owing to the incompatibility between the hydrogel
network and nanofillers. As well, recyclability, biocompatibility, multi-
sensing capacity, and other interesting properties ought to also be
carefully considered. On this basis, the synthesis strategies and design
principles of hydrogel sensors and nanofillers classification are mainly
covered in this review. For that, we first describe how to employ nano-
species such as non-metallic, metallic/MONPs, polymeric, and bio-
nanomaterials as nano-filler to design PVA polymeric hydrogels with
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Advances in Colloid and Interface Science 305 (2022) 102705
tremendous properties that make them appropriate for sensory appli­
cations. These features contain mechanical strength, biodegradability,
biocompatibility, multi-functionality, long-lasting stability, self-
adhesiveness, and so on as shown in Scheme 1. Then, the key ele­
ments assessing an ideal strain/pressure probe have been highlighted in
terms of electronic and ionic conductivity, compressibility, stretch­
ability, fatigue resistance, response time, strain sensitivity, and recovery
time. Lastly, we pronounce some challenges and future directions to
enhance the performance of PVA nanocomposite hydrogel-based
sensors.
2. PVA hydrogel modified NPs in the flexible/wearable sensors
PVA hydrogel-based sensors have been smartly designed and widely
used for the monitoring of human motion and various target bio­
molecules in complex matrices in recent years, which has evidenced
their potential application in flexible/wearable sensing fields. In this
context, a significant number of PVA-based nanocomposites were
established for the highly selective and sensitive determination of
several biomolecules. The extensive application of NPs as functional
membranes or substrates to enhance the signal for scaffolds has been
reported by various researchers in the field of bio-analysis and strain
sensors [38–41]. Herein, a comprehensive summary of related works has
been listed below and shown in Table 1.
2.1. Non-metallic nanomaterials/PVA hydrogel nanocomposites
Carbonaceous nanomaterials including graphene, CNTs, fullerenes
(e.g., C60) have been the most significant and abundant non-metallic
substances affording many remarkable merits owing to their biocom­
patibility, feasible surface functionalization, high stability, high con­
ductivity, extraordinary surface-to-volume ratio, low cost, and strong
mechanical strength [42,43]. Therefore, they have employed and
designed for various promising biomedical applications. The impurities,
edge-plane-like sites, and reactive surface functional groups of carbon
nanomaterials can be accountable for the promotion of their sensing and
tremendous electrocatalytic performances [44,45]. Lots of de­
velopments have been explored on carbon nanomaterials mainly
incorporated into polymers for introducing further functionalities to the
polymers and used in several biomedical applications such as the sensing
field.
CNTs, as a common nano-filler, have gained considerable attention
because of consuming fascinating properties. CNTs are cylindrical tubes
comprising sp2 hybridized graphene sheets that exhibit excellent elec­
trocatalytic ability, electrical conductivity similar to copper, and more
tensile strength than steel. On account of the number of the graphene
layer in the structure of the CNTs, they could be generally classified as
single-walled (SWNTs), double-walled (DWNTs), and multi-walled
CNTs (MWNTs) [46]. In general, their unique physical and chemical
(especially, electrical and mechanical) features improve the perfor­
mance and stiffness of hydrogel-based biosensing platforms [47]. The
excellent mechanical and electrical conductivity properties of the CNTs
arouse from s-orbital and p-orbitals components in the sp2 hybrid
orbital, respectively. Importantly, the CNTs obstacle is their poor solu­
bility or dispersion in inorganic/organic solvents despite their van Der
Waals interactions [48,49]. Hence, the limited coupling interaction
between hydrophobic CNTs and hydrophilic polymers such as PVA
could be addressed by the CNTs surface modification with polar groups
such as amine (NH2), hydroxyl (OH), and carboxylic (COOH) groups
[50]. In CNTs/PVA hydrogel nanocomposites, CNTs can not only be
efficiently introduced to the matrix of PVA; but also shorten the inter­
layer distance resulting in significant nonlinear improvement in me­
chanical properties [51]. In this regard, Chebil and coworkers [52]
fabricated PVA nanocomposite with various weight ratios of COOH-
functionalized MWCNT via solution casting method and characterized
their structural properties. The lowest energy bandgap and a massive
Z. Karimzadeh et al.
Scheme 1. PVA nanocomposite hydrogel-based wearable sensors: employed nano-fillers to design PVA polymeric hydrogels with tremendous properties.
electrical conductivity proliferation were obtained by the use of 5 wt%
of MWCNT which indicates PVA/CNTs nanocomposite as a promising
platform in nanotechnology development. Hydrogels can have excessive
perspective in pressure and strain sensors depending on their tunable
network structure, chemistry, and mechanical properties that are much
similar to the real human skin. Strain sensors could convert mechanical
energy into other types of energy like optical or electrical signals
compared to actuators [53]. Cheng et al. [54] produced a compressible
and stretchable nanocomposite hydrogel strain sensor based on PVA/
MWCNT-COOH/polyacrylamide (PAAm) for detection of human mo­
tion. In this study, the reinforced mechanical and conductive features of
the propounded platform have been assessed in the existence of car­
boxylic functionalized MWCNT as a nanofiller. Due to the existence of
OH groups in PVA chains and abundant COOH groups in MWCNTs, PVA
chains and MWCNTs were cross-linked via the PAAm chains through
plentiful hydrogen bonds as shown in Fig. 1A. SEM images were
considered to further discover the microstructure of the nanocomposite
hydrogel. As illustrated in Fig. 1B, the PVA/MWCNT/PAAm in the
hydrogel has a porous structure, which contains linked sheets with a
thickness of ~200 nm. The assessment of these synergistic effects results
in either excellent self-adhesion ability or high sensitivity/stretchability
of the sensor platform. Although most of the hydrogel based strain
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sensors necessitate external fixation assistance on human epidermal
skin, however, the PVA/MWCNT/PAAm nanocomposite hydrogel
exhibited high tensile strain and compressibility up to 70 % and a broad
sensing range of 500 % without the requirement of any fixation assis­
tance (Fig. 1C, D). Owing to the wide sensing range, the high sensitivity
and the ease of fabrication make them be practically used in personal
health monitoring or sensors. The most significant concern is probable
aggregation of CNTs-hydrogel matrix that limits their efficiency and the
applications of PVA/CNTs hydrogel. So far, enhancement of the CNTs
dispersion in PVA matrix is the main challenge.
Graphene is an extended two-dimensional (2D) carbon material that
has been intensively explored because of its high surface area, great
stability/selectivity/sensitivity, ultra-high electrical and thermal con­
ductivity properties, and excellent electrocatalytic activity [55]. These
sp2 hybridized graphenes could be in different forms of graphene oxide
(GO), reduced GO (rGO), graphene nano-ribbons (GNRs), etc. after
freeing the CNTs. However, few investigations reported pristine
graphene-based materials for tissue engineering, actuators, and bio­
sensors applications. Though, their modified forms and important de­
rivatives like GO with strong oxidizing agents have been widely used
[56]. The presence of abundant hydrophilic oxygenated groups such as
carboxyl, epoxy, and hydroxyl functional groups on the surface of GO
Z. Karimzadeh et al. Advances in Colloid and Interface Science 305 (2022) 102705

Table 1
Classification and summary of PVA nanocomposite hydrogel-based flexible/wearable (bio) sensors.
Nanomaterials Hydrogel Stretchability Sensing types Conductivity Signal Gauge Factor or LOD Ref.

CNTs/PVA PVA/CNTs – Strain sensor (50%) 5.13 3.18 (at 50%) [56]
PVA/MWCNT/PAAm 224.5 % Strain sensor – 4.02 at 300–500 % [54]
F-SWCNT-polyPDAPVA >100% Bending and relaxing of walking, chewing, and – – [176]
pulse sensor; Self-healing; self-adhesive
SWCNT/PVA >1000% Bending and relaxing of knee/finger Sensor – 1.51 [177]
(>1000 cycles); Self-healing
GO/PVA PVA/chitosan/GO – Strain sensor – 1.9 (175% < Δε < 300% [60]
CWCC-rGO/PVA 25% Energy storage sensing material 5.7 μA – [63]
AlgPBA/PVA/PAAM/ – Pressure sensor 0.05 0.11 kPa− 1 (0–10 kPa), 0.015 [178]
rGO kPa− 1 (10–100 kPa)
PVA-chitosan/Rgo – Pb sensing – 0.05 ppb [64]
PC/rGO-PVA >5000% Finger bending, smiling, speaking, and wrist – 14.14 [179]
pulse sensor; elf-healing (~3s)
1
AuNPs/PVA poly(ionicliquids)/ 99% Strain sensor 2.0 Sm− 7.28 MPa [78]
PVA/AuNPs
− 1
AuNPs/PVA – Ceftriaxone sensing – 0.33 μg mL [79]
1
AgNPs/PVA AgNWs/PVA 500% Strain Sensors 1.85 Sm− 0.58) [34]
PVA/AgNPs – Finger and wrist bending, swallowing, and – – [83]
nodding sensor
AgNWs/PVA 350% – 1 × 104 Sm− 1 – [85]
PVA/lignin/Ag NP Strain Sensors 7.1 Sm− 1 – [180]
LM/PVA LM/PVA Strain Sensors 1.3 × 105 Sm− 1
– [97]
LM-Fe2O3/PVA Microelectronic sensors – – [94]
MXene/(PVA) PVA/borax/f-MXene – Gas barrier – Oxygen permeability of 0.73 × [120]
10 2 cc•cm/m2•day•atm
MXene/PVA 1200% Strain Sensors – 0.4 [121]
MXene/PVA/PAM Up to 1200% Strain Sensors Up to 4.25 GF:44.85 [122]
Sm− 1
MXene/PVA/PVP – Strain Sensors – – [181]
MXene/(PVA) >3400% Human speaking, writing, – 25 [182]
and smiling sensor; Self-healing; self-adhesive
MO/PVA ZnO/PVA – Dopamine sensing – 5.0 nM [125]
NiO/PVA/GQDs – Sensing applications; Energy storage – – [130]
Natural Polymer/ PVA/PVP/CNCs – Strain Sensors – 0.478 [183]
PVA PVA/Ag-TA@CNCs >4000% Strain sensors (up to 400%) 4.61 – [154]
2
PVA/ up to 869% Motion sensor 1.75 × 10− S – [153]
tannicacid@CNCs-Rgo m–1
PEDOT/PVA PEDOT/PVA – Motion sensor – – [184]
PEDOT: PSS/PVA 239% Strain Sensors (100%) 0.36 S.m− 1 4.4 [173]
PEDOT: PSS/EG/PVA – Strain Sensors (20%) 26±1.5 % – [172]
PEDOT: PSS/cellulose/ – Strain Sensors 0.3 S.cm− 1 – [175]
PVA
PANI/PVA PANI/PVA – human movements – 4.28 [167]
PANI/PVA/PAA – Strain Sensors – – [166]

nanosheets enable their feasible and uniform dispersion in water and
many other solvents using physical interactions and hydrogen bonds
[57]. Noticeably, these superb properties make graphene an ideal
candidate to be used in either flexible electronic devices for attaining
high-performance sensors and actuators in biomedical applications or
negative permittivity (i.e., the ε-negative materials) [58]. To date, gra­
phene has been widely considered as an efficient filler, physical cross-
linker, energy converter, and efficient enforcement not only in high-
performance sensors based on nanocomposite hydrogel [59]; but also
in shape memory hydrogels [60]. In shape memory hydrogels, the
deformed shape could be fixed then its original shape is restored under
external stimuli such as solvent, ultrasound, pH, and temperature. In
addition, the distinctive stretching hydrogel platform with controllable
shape memory properties demonstrates promising potential in biolog­
ical devices and wearable/flexible electronics by efficiently prolonging
the service life [61]. However, the oxidized form of graphene strictly
reduces the electrical conductivity and disrupts the conjugated struc­
ture. GO could be integrated into hydrophilic polymers chemically or
physically to form cross-linking networks. In the place of PVA polymer,
the preparation of GO/PVA hydrogel nanocomposites is through
hydrogen bonding with improved conductivity, tensile fracture
strength, self-healing ability, and mechanical performance capabilities
[62]. Recently, the development of PVA hydrogel sensor with remolding
performance and shape memory is still essential for the multi-field
application. In this regard, Yang et al. [60] fabricated a physically
cross-linked shape memory hydrogel sensor with the integration of PVA,
chitosan, and GO and employed as a wearable strain sensor. As shown in
Fig. 2A, PVA bonded with glycerol through hydrogen bonding, whereas
GO and chitosan were cross-linked over electrostatic interactions
forming a hydrogel network. The hydrogen bonds in PVA molecular
chain provide the thermo-responsive shape memory sensor that regains
its orientation after heating. Following Fig. 2B, these great properties of
shape memory hydrogel sensors triggered this nanocomposite hydrogel
to be integrated into temperature measurement devices. The hydrogels
can efficiently dissipate energy and rebuild the network on account of
the dual physical cross-linking that finally reached remolding properties
and excellent strength. Likewise, the chitosan introduction grants the
outstanding electrical conductivity of the platform to be involved in
strain sensors. Additionally, the stress-strain curves with different
weight ratios of cationic chitosan (increasing from 5 to 15 wt%) indi­
cated an increase from 1.0 to 1.6 MPa, as shown in Fig. 2C. However, the
decrease in toughness and tensile strength at a higher ratio of chitosan
could originate from the formation of the less stable structure due to
inhomogeneity caused by introducing high content of cationic chitosan
and a physically cross-linked network of PVA. Inspired by the results, the
designed PVA/chitosan/GO nanocomposite hydrogel perfectly explored
its application in subtle motion (vibration of the throat) and large mo­
tion (joint movements) of humans (Fig. 2D).

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Fig. 1. Represented illustration for the preparation process of the PVA/MWCNT/PAAm nanocomposite hydrogel (A); SEM images of the nanocomposite hydrogel in
which MWCNTs are designated by the red arrows (B); Stretching, compressing, and high toughness of nanocomposite hydrogel (C and D). Reproduced with
permission from [54].

Additionally, Xiong et al. [63] have designed carbonized wood cell
chamber-rGO/PVA (CWCC-rGO/PVA) nanocomposite hydrogel with
high sensitivity, reasonable stress resistance, shapeable structure, high
flexibility, and high specific capacitance. As shown in Fig. 3A, briefly,
the rGO-CWCC composite was prepared by mixing the GO with
carbonized CWCC. Then, the PVA-based nanocomposite hydrogel was
obtained through a spin coating procedure and ultimately used in the
moisture-electric generation, strain sensing, and energy storage appli­
cations. PVA contributes to either sensitive sensing properties for
detecting physiological signals of human movement or the high
deformability and flexibility of the nanocomposite hydrogel depending
on the abundant free protons in PVA (Fig. 3B). Since the prepared hybrid
holds many hydrophilic groups such as -OH, it is represented that
hydrogen bonds are formed between water and nanocomposite hydrogel
when contact with moisture. As depicted in Fig. 3C, the movement of H+
from the high-concentration region to the low-concentration one
generated the electrical current. Also, the introduction of GO as inter­
mediate material was for C-C binding to CWCC and hydrogen binding
with PVA. In terms of sensing, the resultant features endow the CWCC-
rGO/PVA nanocomposite hydrogel to be used as portable or wearable
electronic equipment to discover physiological signals of human motion.
In another work, Nguyen and coworkers [64] fabricated an eco-

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Z. Karimzadeh et al.
Fig. 2. Schematic mechanism of the hydrogel formation (A); The temperature-responsive shape memory behavior of PVA/chitosan/GO nanocomposite hydrogel (B);
The stress-strain curves for the different ratio chitosan in nanocomposite hydrogel (C) and function of the strain hydrogels, cyclic test, relative resistance changes on
the neck and finger (D). Reproduced with permission from [60].
friendly and effective platform based on PVA-chitosan and rGO nano­
composite hydrogel for electrochemical determination of lead (Pb) in
real water samples. For that, the GO was synthesized from an eco-
friendly thermal exfoliation-reduction process that exhibited increased
electron transfer benefiting from their outstanding electronic properties.
Besides, the high amount of loading target was a result of their large
surface area. For further improvement of chemical and mechanical
properties, chitosan as a common copolymer [65,66] was blended with
PVA in which the enhanced properties are possibly attributed to the
PVA-chitosan interaction through intermolecular, intramolecular, or
hydrophobic side-chain hydrogen bonds. The obtained well-dispersed
and homogeneous nanocomposite hydrogel platform demonstrated a
low limit of detection (LOD) of 0.05 ppb and linear detection range
(LDR) of 1–50 ppb.
2.2. Metallic nanomaterial/PVA hydrogel nanocomposites
Metallic NPs including palladium (Pd), platinum (Pt), silver (Ag),
gold (Au), and their core-shell NPs or bi/trimetallic alloys are essentially
fascinated by numerous biosensing or bioimaging applications by virtue
of their several intriguing electrochemical, chemical or physical (shape/
size) merits such as enhanced electron transfer, catalytic properties, ease
of surface functionalization and facile synthesis [67–70]. Currently,
biosensor platforms based on metal NPs afford great potential for
enhancing selectivity and sensitivity through adjusted signal amplifi­
cations [71–73]. Regarding the beneficial advances in their design, bio-
functionalized NPs and effective nanocomposites such as hydrogel
nanocomposites are extensively investigated in several analytical ap­
proaches, drug delivery, conductive scaffolds, and biosensors applica­
tions. Incidentally, metal NPs are embedded in the polymeric networks
for further diverse characteristics derived from loading different kinds of
NPs [74]. Nevertheless, strong dipole-dipole attractions and the high
surface energy among metallic NPs prevent reaching a stable dispersion
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in an aqueous solution. This issue could be well addressed by the
development of two main synthesis methods. First is the growth of nano-
species inside the hydrogel network from a seed-precursor. The second is
producing hydrogel with free-radical polymerization using reactive
metallic NPs as cross-linkers [75]. The second method results in
hydrogel nanocomposite with high mechanical strength due to strong
interfacial interactions compared to the first method.
Specifically, AuNPs offer outstanding sensing and biosensing pros­
pects due to beneficial aspects of great catalytic activity, widespread
electrochemical potential range, high biocompatibility, high chemical
stability, easy fabrication, and surface modification process [76]. Based
on the aforementioned properties, AuNPs can serve as the miniaturized
sensing devices to the nanometer scale, which proposes exceptional
prospects for chemical sensing [77]. For improving the reproducibility
and stability of the sensor platform, they are incorporated into the
hydrogel matrix. The AuNPs as conductive material explored their
application in the fields of sensors benefitting from synergic key prop­
erties of polymers and NPs. In this regard, He et al. [78] have reported a
facile way of fabricating AuNPs-embedded PVA nanocomposite hydro­
gel with excellent electrical and mechanical self-healing properties
making it potentially suitable for a variety of applications. For that, dual
network hydrogel was prepared using physical and chemical cross-
linking as shown in Fig. 4A. To increase the conductivity of the com­
posite, AuNPs have been selected and reduced in-situ as conductive
fillers without the presence of any reductant. Both 1-methyl-3-(4-vinyl
benzyl) imidazolium chloride P(VBIm-Cl) and sodium p-styrene sulfo­
nate hydrate (NaSS) as poly (ionic liquids) were incorporated into the
PVA network in the presence of N, N′ -methylene bis acrylamide as a
cross-linking agent. The coordination effect between the hydroxyl group
and AuNPs and hydrogen bonds between -OH sides groups lead to the
self-healing ability of the developed hydrogel. Conductive behavior and
conductive function self-healing behavior of the nanocomposite hydro­
gel were investigated using conducting electronic circuit of LED at room
Z. Karimzadeh et al.
Fig. 3. Illustration of the formation process of the CWCC-rGO@PVA composite and chemical bond between rGO and PVA in CWCC-rGO@PVA (A); Human signal
strain sensing test (B); The mechanism, by which moisture generates electricity (C). Reproduced with permission from [63].
temperature. The electrical performance of the original hydrogel,
broken hydrogel and self-healed hydrogel obviously indicated that
intrinsic conductivity was restored after the broken hydrogel was self-
healed (Fig. 4Ba–c). The obtained poly (ionic liquids)/PVA/AuNPs
nanocomposite hydrogel exhibited repeatedly restoring in which con­
ductivity and self-healing properties were almost unchanged. The results
illustrated that the designed PVA hydrogel could experience gel-to-sol
transition due to the reversibility of Au-OH coordination that is appro­
priate to form a gel with different shapes.
In another effort, Pourreza et al. [79] fabricated a nanoprobe based
on AuNPs/PVA nanocomposite hydrogel for colorimetric determination
of ceftriaxone in spiked urine and plasma samples. Briefly, PVA polymer,
borax, and HAuCl4 were mixed and the final nanocomposite hydrogel
was prepared in one-pot and in a short time. In this study, the presented
PVA template has the advantage of its similarity to the biological matrix
to be used in analytical chemistry and biological fields. The borax-cross-
linked PVA hydrogel network act not only as a reducing agent for
simultaneous loading and synthesis of the AuNPs; but also as a sensing
platform. This PVA-AuNPs hydrogel was adequately used for selective
and sensitive determination of ceftriaxone. Since the AuNPs have the
ability to attach the -SH than -NH functional groups, this platform could
be explored for ceftriaxone monitoring possessing -SH groups. A two-
step cross-linking mechanism (mono-diol and di-diol complex) has
been proposed for the formation of hydrogel between PVA and borax as
illustrated in Fig. 5. The forming or expansion of hydrogel was due to
electrostatic repulsion among these two stages [80]. Furthermore, the
obtained PVA-borax network was responsible for the in-situ formation of
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Advances in Colloid and Interface Science 305 (2022) 102705
AuNPs. The reducing -OH groups in PVA hydrogel reduce the Au3+ ions
to AuNPs in alkaline media. Importantly, the obtained hydrogel network
could possibly avoid the aggregation of AuNPs during the reduction
process. Finally, at ambient conditions, the low LOD of 0.33 μg mL− 1 and
wide LDR of 1–90 μg mL− 1 were obtained for ceftriaxone. Therefore, the
results for the performance of the platform were satisfactory.
Alternatively, AgNPs have aroused scientific interest owing to high
biocompatibility, amplified electrochemical signals, and excellent con­
ductivity. Moreover, AgNPs exhibited tremendous antibacterial activity
against Gram-negative and Gram-positive strains making them essential
for sensing biomedical platforms. This antibacterial activity could be
originated from the interactions of -S groups of bacterial proteins with
Ag ions causing protein damage and electron transport interrupt [81].
To date, massive efforts have been made toward the construction of Ag-
based nanocomposite with polymers such as PVA leading to enhanced
stability, electrical conductivity, high swelling/deswelling rates, and
biosensing performance despite the comprehensive utilization of the
materials [82,83]. The dispersion manner and preventing aggregation
are two processes that outline the stability and sensitivity of the AgNPs
in the PVA network. AgNPs could be stabilized through electrostatic and
steric repulsion of the stabilizing agents with the polymeric matrix.
Since PVA high concentration is essential for achieving high mechanical
strength, conductive NPs could be well dispersed in PVA solution with
low concentration [84]. For addressing this issue, Azadi and coworkers
[34] designed highly stretchable and biocompatible Ag based PVA
hydrogel strain sensors for the detection of human motion. The proposed
bilayer platform had a highly conductive layer of AgNWs/PVA that was
Z. Karimzadeh et al.
Fig. 4. Preparation procedure of the PVA@Au nanocomposite hydrogel (A); Conductive function and self-healing behavior (B) of original hydrogel (a), broken
hydrogel (b), and self-healed hydrogel (c) at room temperature. Reproduced with permission from [78].
supported by a tough PVA substrate layer as shown in Fig. 6A. The high
mechanical property assigned from the viscose layer of PVA, meantime,
their high electrical conductivity could be obtained from better disper­
sion of AgNWs in the low viscose PVA layer. The main piezoresistivity
mechanism including the disconnection between AgNWs and increased
interparticle distance upon stretching in Fig. 6B demonstrated high
stretchability up to 500% strain for PVA nanocomposite. To analyze
attachment and spread of fibroblast on the PVA based substrates, cell
morphology was considered. According to Fig. 6C, a successful attach­
ment and well-spread morphology were observed for immunostained
fibroblasts in control (polystyrene), PVA, and PVA/AgNWs substrates.
Also, the high electrical conductivity of 1.85 Sm− 1 and mechanical
strength of 900 kPa were obtained with excellent LDR. These features
have unlocked up the opportunity of the proposed sensor as a wearable
sensor for monitoring human motion (Fig. 6D).
Furthermore, Wang et al. [85] incorporated porous and stretchable
AgNWs/PVA nanocomposite hydrogel with CNTs electrodes and devel­
oped flexible tactile sensors. Various human motions were determined
with an eco-friendly wearable sensor with significant stability of 10 000
loading/unloading cycles, a quick response time of 25 ms, a wide
detection range of 250 kPa, and high sensitivity of 1.9 kPa− 1. These
PVA-based nanocomposite hydrogels have been directed toward the
development of small sensor devices with desired shapes.
In the light of the manufacturing of nanocomposite hydrogels, a
contradiction occurs between the degree of dispersion and nanofiller
loading due to Coulomb and van der Waals attractions that affect their
performance. Thus, the homogeneous dispersion and amalgamation of
fillers in the polymeric matrix are extremely challenging. The difficulty
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over the dispersion and loading control has frequently prohibited
nanocomposites from achieving multi-functional necessities. This mat­
ter has been accentuated in the field of wearable and flexible soft sensors
such as skin or epidermal sensors. Generally, epidermal wearable sen­
sors suffer from tearing and puncturing which leads to poor electrical
and mechanical performance [86]. Using conductive hydrogel with
different rigid conductive fillers such as non-metallic, metallic/MONPs,
polymeric, and bio-nano materials has been explored its application in
constructing wearable epidermal sensors [87]. However, the rigid
property of the aforementioned conductive fillers could bring about
mechanical resistance with the soft hydrogel leading to internal stress
concentration. Among these rigid materials, liquid metal (LM) NPs have
particularly sparked a new class of soft fillers with a tunable and unique
set of features.
2.3. LMs/PVA hydrogel nanocomposites
LMs are multifunctional flexible and soft metals or metal alloys that
are liquid at room temperature. LMs offer amazing potential for elec­
tronic, sensing, and catalytic applications because of their high electrical
conductivity and fluidic compliance that possess an interface with access
to electrons and free ions [88,89]. LMs could be incorporated inside
sense strain and polymeric materials by calculating resistance change
arising from the LM deformation during the bending, twisting, and
stretching. Seminal efforts have focused on nanosized LM that indicate
high surface tension, leading to improvement in dispersibility inside a
polymer matrix [90]. Particularly, LM fillers possess tunable and unique
sets of properties attained via selective alloying of LMs with metallic or
Z. Karimzadeh et al.
Fig. 5. Schematic presentation of nanoprobe based on AuNPs/PVA nanocomposite hydrogel and their corresponding TEM images for colorimetric determination of
ceftriaxone. Reproduced with permission from [79].
other elements [91,92]. These NPs perform as a resistance-less liquid
that could bend and deform under stress with no mechanical damage or
delamination in composite matrix compared with traditional conducting
materials [93]. In terms of strain and digital electronics, these circuits
show lower electromechanical hysteresis and smaller gauge factor (GF)
than conductive rigid filler. Alloys of indium (In), gallium (Ga), and
eutectic Ga-In (EGaIn) are the most popular conducting LM alloys for the
expansion of soft and flexible electronics. However, their poor surface
wettability and excessive surface tension limit the large-scale applica­
tion of LMs. To overcome these shortcomings, various schemes have
been proposed. Mixing LM NPs with various elastomers such as silicone,
agarose gel, PVA, and polydimethylsiloxane is one of the approaches to
improve the uniform dispersion and recyclability of LMs [94]. In most of
these inert elastomer materials, the incorporation of LM NPs results in a
loss of electrical conductivity due to both typical nonconductive poly­
mer matrices and the construction of a thin oxide layer on the NPs
surface [95]. Among them, PVA-based hydrogels present the advantage
of electrochemical/electronic improvement and LM NPs stabilization.
The PVA network can mitigate the loss of electrical conductivity of the
LM filler due to the unavoidable alignment of a surface oxide layer.
Furthermore, the surface interaction between the functional -OH group
on the PVA and the surface oxide skin layer of LM NPs can also form a
conductive ionic junction that stabilizes the LM NPs [96]. Considering
these belongings, Xu et al. [97] developed a recyclable compounding
strategy based on PVA/LM composite with improved surface wettability
and low surface tension of the LMs (Fig. 7A). Here, PVA/LMs matric with
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a volume ratio of 10:1 has been fabricated via a simple method of
dispersing PVA solution in LM for 5 min. Surface wettability was
improved since PVA solution performed as a bridge between substrates
and the surface oxide film. Moreover, it has been proven that PVA hel­
ped the bulk LMs disperse into uniform nanosized particles under high-
speed dispersion. At this state, the achieved PVA/LM ink holds enhanced
processability than the pure LMs facilitating their recovery without
aggregation. The admirable conductivity and electrical properties of
PVA/LM ink are favorable for designing flexible sensors, alarm systems,
or object locators to monitor human motions as illustrated in Fig. 7B. In
strain sensors, the obtained eco-friendly composite had super stability
and high sensitivity which can sense the signal from stretching, bending,
and pressing. Also, LMs in printed products could be recovered and
reused under alkaline conditions making them an eco-friendly system to
be used in flexible electronics.
To broaden its wide application, Merhebi and coworkers [94]
fabricated conductive and magnetic LM/PVA gels that were potential for
flexible electronic system design. The schematic presentation of the
cross-linking mechanism was illustrated in Fig. 8. Herein, EGaIn alloy
was integrated into the magnetic solution of Fe3O4 particles and finally,
PVA was processed into NPs with an average size of 140 nm followed by
sonication which indicated cubic to octagonal symmetries, as exposed in
the SEM images (Fig. 8A). The degree of hydrolysis and molecular
weight of the PVA chains that are produced from the hydrolysis of poly
(vinyl acetate) (PVAc) can affect their microstructure and physical
characteristics. In this work, the PVA with a 99% degree of hydrolysis
Z. Karimzadeh et al.
Fig. 6. Design and fabrication process of AgNWs/PVA hydrogel bilayer strain sensor (A); piezoresistivity mechanism indicating disconnection of AgNWs and
increased interparticle distance (B); Fluorescent images of PVA, and PVA/AgNWs substrates captured by fluorescent and confocal microscope (upper and lower
panel) (C); Monitoring the human motions and relative change in their resistance (D). Reproduced with permission from [34].
which was the reason for mechanical properties provides enhanced
compatibility with the inorganic additives via hydrogen bonding. For
producing multifunctional self-healing and flexible gel, the dynamic
borax cross-linking reaction was performed within inter and intra-
molecular domains as clarified in Fig. 8B, C. Moreover, molecular
chains were further linked together via diol complexation reactions and
weak hydrogen bonds by -OH groups on the PVA microstructure.
Complexation and oxidation reactions between the LMs and Fe3O4
particles were assessed by FT-IR, XRD, and Raman studies. The obtained
LM/PVA gel was applied as an electrical switch, in which the electronic
circuit was remotely closed by the magnetic field. This progress has
unlocked up the opportunity for the design of soft electronic systems.
2.4. 2D materials/PVA hydrogel nanocomposites
2D nanomaterials could be alienated from bulk solids consisting of
atomically thin layers in the out-of-plane direction by van der Waals
forces. Thin and few-layer nanosheets are characterized by active, large
surface area and diverse electronic character that is favorable for sensor
applications [98–100]. The booming 2D materials, signified by gra­
phene, resulted in a number of prospects to construct multifunctional
composites [101–104]. Recently, novel 2D nanofillers beyond graphene
have been introduced including transition metal dichalcogenides
(TMDs) [105], transition metal carbides and nitrides (MXene)
[106–108], metal-organic frameworks (MOFs) [109,110], and hexago­
nal boron nitride (h-BN) with distinct robustness and mechanical flexi­
bility. Polymer nanocomposites composed of 2D nanofiller and polymer
matrix are pivotal materials for various developing technological fields
of sensors arising from the 2D material properties. Nevertheless, using
conventional synthesis design and approaches to the assembly of 2D
materials with spatial distributions and controllable orientations in
polymers is challenging [111]. These 2D nanomaterials are also limited
in high content to attain homogeneous dispersions without accumula­
tion in a polymer matrix. Therefore, transforming the conventional
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complexes into multifunctional ones and fully translating the
outstanding properties of 2D nanofillers into composite constructions
are the two ultimate goals. At this state, rational assembly techniques of
2D fillers through altered length scales facilitate their controllable
alignment, interconnection, and dispersion in a polymer matrix [112].
Such assembly methods bring about inspiring transformative nano­
composites with promising electromagnetic, optical, mechanical, and
transport features. At the nanoscale, synthesis techniques including CVD
growth on metal templates and liquid-phase exfoliation of bulk crystals
play crucial roles in the inherent properties of 2D fillers [113]. Among
various 2D counterparts, MXene and TMDs as two so-called materials
have aroused much scientific interest in fabricating nanocomposites
[114,115]. 2D MXene (Ti3C2Tx) was introduced by Gogotsi’s group in
2011 for the first time [116]. 2D MXene-based sensors are nanosheets
with a wide sensing range and great flexibility resulting in fabrication on
a large scale and decoration of various shapes. On account of
manufacturing ideal sensors, realizing mechanical performance well-
matched with sensitivity, stability, conductivity, rapid and on-site
analysis in the extensive range is the most prominent matter for
MXene-based sensors. To solve these challenges, seminal efforts have
been applied. For green and economical synthesis fluorine-free reaction
systems are interested to be used in order to yield large-scale production.
From the point of performance stability, the antioxidant ability of
MXene is not ideal in a water and oxygen environment. To date, diverse
functional substrates are considered to incorporate with conductive
MXene to attain admirable sensing proficiency preferred in the
controllable multidimensional sensors. Benefiting from the high con­
ductivity, MXene could be integrated into a water-rich cross-linking
hydrogel for the development of compatible sensors and implantable
devices with tremendous elastic modulus analogous to real human skin
[117]. Such high content of water enables good dispersibility of MXene
in hydrogel matrix because of their hydrophilic surface groups (-F, -Cl,
-Ti, -O, and -OH) [118]. Furthermore, the structural design MXene/
hydrogel is beneficial for high sensitivity though avoiding the possible
Z. Karimzadeh et al.
Fig. 7. Fabrication, printing, and recycling process of the LM/PVA and diverse patterns printed using LM/PVA ink (A); Applications of the LM/PVA based flexible
electronics in motion monitoring (B). Reproduced with permission from [97].
aggregation of MXene flakes during the preparation process achieve
through hydrogen bonding and Van der Waals attractions [119]. PVA as
a flexible substrate catches the spotlight because of its tensile strength
and excellent stretchability. Woo et al. [120] fabricated PVA/borax/
MXene nanocomposite hydrogel and investigated the effects of borax
addition on their physical properties. In this study, MXene reinforcing
filler was functionalized with the sulfanilic acid group (f-MXene) via
diazonium salt reaction. As shown in Fig. 9A, Ti3AlC2 was dispersed in
HF solution followed by washing and drying at room temperature. After
obtaining DMSO-intercalated MXene, f-MXene was prepared using sul­
fanilic acid addition. According to Fig. 9B, such functionalization
induced homogeneous dispersion. Afterward, PVA functionalized
MXene nanocomposite hydrogel was fabricated by directly mixing
MXene, borax, and PVA solution. The borax cross-linkers in Fig. 9C
created strong interfacial covalent bonds between the hydrophile PVA
matrix and the f-MXene reducing the surface tightness of a single-layer
MXene sheet. Furthermore, Fig. 9D illustrates the mechanical properties
for f-MXene loading which indicates increase in tensile strength by
increasing the filler content. Indeed, f-MXene acts as a promising rein­
forcing filler to increase the mechanical properties of the PVA nano­
composites. This strategy helps the formation of robust PVA/boric acid/
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MXene nanocomposite films with improved mechanical properties,
thermal stability, and oxygen permeability. In optimum conditions, an
increase in initial thermal decomposition temperature from 257.4 to
288.2 ◦ C was exhibited. Also, tensile strength and modulus were
improved by 67% and 49%, respectively. These outcomes obviously
propose a practical platform with improved properties in proficient gas
barrier film applications.
In another work, Zhang et al. [121] utilized almost the same protocol
as Woo group [120] for the fabrication of capacitive strain sensors using
PVA/MXene hydrogel. The prepared nanocomposite demonstrated
linearity up to 200%, great electrical conductivity, a sensitivity of 0.4,
and a high break elongation of 1200% because of its excellently
stretchable capability that is feasible for wearable intelligent devices. In
this regard, the developed sensor is not only used to determine
epidermal movements but also large-strain movements. Nevertheless,
the low response time of 190 ms needs to be enhanced in upcoming
investigations.
On the other hand, the conventional conductive hydrogels partici­
pate in the unavoidable freeze at subzero temperatures and loss of water
at room temperature; because they are composed of lots of water. This
limited the electron transference in the network leading to a decline in
Z. Karimzadeh et al.
Fig. 8. Preparation procedure of the conductive and magnetic LM/PVA nanocomposite hydrogel: illustration of PVA, Fe3O4 nanopaticles (220 nm), and EGaIn and
sonication process to micronize LM into nanosized particles (A), gel formation by borax cross-linking reaction (B), and mechanism of cross-linking (C) with mono-diol
(i), di-diol complexation (ii), and hydrogen bonding (iii). Reproduced with permission from [94].
mechanical and conductivity properties. To avoid this, Liao and co­
workers [122] designed PVA/MXene/PAAm-based strain sensors with
high stretchability, elasticity, sensitivity, and low-temperature toler­
ance. In this study, borax cross-linkers were added to the completely
dissolved and initiated PVA, MXene, and PAAm solution. For achieving
durable retention ability and excellent frost residency at low tempera­
tures, MXene-based PVA hydrogel was immersed in ethylene glycol (EG)
solution to substitute a part of water content. Fig. 10A represents the
replacement of water molecules in the hydrogel by EG molecules and the
formation of hydrogen bonds between PVA, EG, and MXene. Also, the
well-exfoliated ultrathin MXene nanosheets and a three-dimensional
(3D) interconnected porous microstructure in nanocomposite hydrogel
were represented in SEM images represented in Fig. 10B–D. The pro­
posed method represented excellent mechanical and chemical proper­
ties with the accurate, sensitive, and durability-sensing ability with a
detection sensitivity of GF = 44.85 and a wide range of sensing (350%)
at low temperatures. Here, the addition of a brittle PAAm network had a
positive effect on increasing the elastic modulus. Moreover, the obtained
hydrogel possessed a self-healing capability owing to the supramolec­
ular interaction among MXene, PVA, and EG and dynamic cross-linking
between borax ions and the -OH groups of PVA. Therefore, the emerging
MXene-based hydrogel sensor suitably meets the required properties of
hydrogels in the fields of human-machine interfaces and artificial skin.
2.5. MONPs/PVA hydrogel nanocomposites
MONPs as marvelous materials in materials science could be formed
from metal elements by chemical methods. The high density of edge
surface sites or corners and limited size of MONPs can extensively result
in distinctive chemical and physical properties. Thanks to their large
surface area, tremendously reduced dimension, and specific facet
exposure, MONPs may considerably improve selectivity and sensitivity
[123]. The integration of MONPs into polar organic polymers inspires
many alterations in polymer catalysis, electronic and optic perfor­
mances. Based on, various MONPs such as iron oxide (Fe2O3) NPs, nickel
oxide (NiO) NPs, titanium oxide (TiO2), zinc oxide (ZnO), manganese
oxide (MnO2), and copper oxide (CuO) have been employed in polymers
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for promoting their efficiency. In this regard, the fabrication of PVA
hydrogels with MONPs has been widely interested.
ZnO NPs found in whitish appearance and wurtzite structure play a
prominent role in various sensory applications because of their low cost
and belonging to the semiconductor group (II-VI). ZnO NPs as electrical
conductors are suitable materials for manufacturing ultrasonic trans­
ducers through owing huge piezoelectric constant. Equipping this
semiconductor with special electrical, optical, thermal, and chemical
properties make them a multifunctional material to be used in various
electronic appliances [124]. ZnO NPs need to be modified as their dis­
persions are prone to aggregate in solution or composite matrix. One
strategy for stabilizing the particle dispersion is the modification of their
surfaces by tethering polymeric chains due to the compatibilization ef­
fect provided by polymeric ligands. The synthetic techniques for the
fabrication of polymer-MO nanocomposites can be divided into two
aspects of surface functionalization and preparation of MO/polymer
hybrids. The concept of surface functionalization mainly focused on the
ready modification of ZnO by different efficient anchoring molecules
such as polymer ligands and coupling agents through their slow disso­
lution in both basic and acidic media. For the preparation of MO/
polymer hybrids, three methods of grafting-onto, grafting-from, and
polymer template are applied. In this regard, ZnO-dispersed PVA com­
posites are the better choice in electronics that brings forth excellent
physiochemical properties. Emadoddin et al. [125] developed a func­
tional pH-inducible ZnO/PVA composite via an electrochemical depo­
sition method for selective dopamine determination in the existence of
ascorbic acid as an interference. As shown in Fig. 11, functional groups
of PVA provide a substrate for functionalization with ZnO, which was
utilized for electrocatalytic dopamine oxidation, and minimization in
surface interactions with fouling agents or interferences. The pH-
inducible property of the ZnO/PVA composite hydrogel provides
fouling-free effects under controlled conditions. Impedimetric assess­
ments of the designed recognition element indicated a low LOD of 5.0
nM and a broad linear range of 20.0 nM-3.0 mM for the determination of
dopamine in real serum samples. The ZnO/PVA composite hydrogel
provides potential goals for sensitive and selective determination in the
presence of ascorbic acid interference besides preventing surface
Z. Karimzadeh et al.
Fig. 9. Schematic synthesizing of f-MXene using diazonium salt reaction (A); Dispersion stability of f-MXene and e-MXene with 1 mg/mL concentration (B); PVA,
boric acid, and f-MXene cross-linking reaction by a di-diol complexation reaction (C); The mechanical properties of f-MXene based nanocomposite hydrogel with
different amounts of f-MXene (D). Reproduced with permission from [120].
fouling. Additionally, the employment of the nondestructive impedi­
metric evaluation method afforded small signal amplitude and a wide
frequency range that is suitable for the investigation of interfacial redox
reactions.
With recent advances in the design of sensors, it is proven that sen­
sors can be influenced not only by sensing structure but also depends
largely on the sensing film employed on the surface of optical fiber
sensors, mainly for humidity sensing. For that, optical fiber surfaces are
often coated with humidity sensing film to distinguish environmental
factors [126]. Electrospinning is a coating method for nanofiber films
different from traditional ones including physical vapor deposition
(PVD), chemical vapor deposition (CVD), layer-by-layer, and dip-
coating techniques [127]. To produce micro/nano-scale nanofibers by
electrospinning, high voltages are applied to polymer solutions which
then can form nanofiber film with a great specific surface. Inspired by
that, Deng et al. [128] recently proposed optical ZnO/PVA nanofiber
film using an electrospinning technique for temperature and humidity
sensing. For guaranteeing the sensitivity and mechanical strength, the
proposed nanofiber was attached to the peanut-shaped structure. As the
thickness and refractive index of sensing film were affected by the hu­
midity changes causing variations in the transmitted light, temperature
and humidity were monitored by evaluating these spectrum changes.
Experimental results exhibited high temperature and humidity
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sensitivity of 11.14 pm/◦ C and − 0.02539 dB/%RH, individually.
Compared with fiber sensor using a PVA film alone, nearly four times
enhancement was exhibited in sensor sensitivity by the addition of ZnO
to the PVA film. On the other hand, Fe2O3 NPs and NiO NPs are proper
MONPs for producing the film, magnetic nanomaterial, and poly­
morphism study which aim for attractive applications in various sensors.
The large band gap of both NiO (3.6–4.0 eV) and Fe2O3 (2.0–2.2 eV) NPs
make them potential materials to be doped in PVA polymers which is a
fixable insulator with a wide band gap. NiO NPs are p-type semi­
conducting materials with outstanding properties of optical, electrical,
and chemical stability. The variation in NiO NPs charge carriers could
change the electrical conductivity. The non-stoichiometric effect of NiO
NPs originated from variation in NiO structures making them prospec­
tive for sensing applications [129]. In this state, Kumar and coworkers
[130] studied morphology and structure of the NiO/PVA nanocomposite
hydrogel which was modified with graphene quantum dots (GQDs) by
the solution casting technique. The synthesis protocol of the nano­
composite is presented in Fig. 12A. The incorporation of NiO NPs in the
polymer network enhanced both thermal stability and tensile strength.
To analyze the interaction between different molecules of the composite,
an Independent Gradient Model (IGM) analysis was carried out, and the
obtained results are presented in Fig. 12B, C. Studying their electronic
structure reveals that the PVA interacts with GQDs indirectly through
Z. Karimzadeh et al.
Fig. 10. Fabrication methodology of a self-healing, anti-freezing, and conductive MXene nanocomposite organohydrogel (A). SEM images (B) of delaminated MXene
sheet (a), and the freeze-dried MXene nanocomposite hydrogel (b, c). Reproduced with permission from [122].
the NiO (Fig. 12C) which is favored in interaction energy terms
compared with the direct interaction of PVA with GQDs (Fig. 12B).
Therefore, the enhancement in the mobility of electrons within NiO/
PVA nanocomposites makes them the most promising materials.
2.6. Bio-nanomaterials/PVA hydrogel nanocomposites
DNA as functional materials have demonstrated excellent potential
for fabricating artificial constructions owing to their programmable and
predictable sequence-specific hybridization with their complementary
sequences (CS) [131]. Among several functional DNA structures, DNA
hydrogels merging the properties of hydrogel and DNA building blocks
have been particularly developed in extensive biomedical and bio­
sensing applications [132]. To construct DNA hydrogels, functional
DNA is either entangle physically or link chemically within the hydro­
philic polymer networks. In the process of fabricating chemical gels,
cross-linking agents and other substances are typically required to be
introduced due to a time-consuming process. Meanwhile, it usually has
no need for external substances in physical gels owing to the simple
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gelation process. Among, physical entanglement could simply respond
to the external environment like temperature and pH, which have
certain benefits [133]. DNA hydrogels have been effectively adopted as
two kinds of pure DNA hydrogels and hybrid DNA hydrogels which are
formed by the cross-linking of DNA backbones itself and in combination
with different materials, respectively. One of the simple procedures to
fabricate DNA hydrogels via cross-linking or self-assembly is the poly­
merization of DNA motifs such as a three/four-way junction. Moreover,
other diverse methods namely hybridization or polymerase chain reac­
tion can enhance the process [134]. In light of the featuring DNA
hydrogel with the additional capability, various functional components
and DNA entities such as nanomaterials, peptides, DNAzymes, or
aptamers could be introduced into the hydrogels [135]. The recognition
of analytes using these surface motifs on hydrogels stimulates the
response and physiochemical sensing characteristics of DNA hydrogels
such as optical, mechanical, volume, and cross-linking density proper­
ties. Endowed with modifiable mechanical properties, controlled
biodegradability, great biocompatibility, and stimuli-responsive
behavior, DNA hydrogels have been adapted as promising platforms in
Z. Karimzadeh et al.
Fig. 11. Illustration of the fabrication process of ZnO/PVA nanoplatelets. Reproduced with permission from [125].
biosensing applications [136]. As far as their applications, hydrogel
cross-linked with aptamer is mostly developed for qualitative and
quantitative detection of various targets. Aptamer as a short single-
stranded RNA or DNA has grown rapidly because of its prosperous ad­
vantages. In the presence of targets, aptamers can not only bind to them
by specificity and high affinity but also fold into secondary and tertiary
structures. Generally, aptamers can integrate into both pure and hybrid
DNA hydrogels by acting as cross-linker or as part of branched DNA
molecules [137]. More in deep, Wang et al. [138] fabricated a PVA/
polyaniline (PANI)/aptamer-based sensor for thrombin detection with
excellent electrochemical and mechanical properties. In this study, the
platform was prepared by the electrochemical copolymerization of 3-
aminophenyl boronic (ABA) and aniline on a PANI modified electrode
followed by dipping in PVA solution. Benefitting from the characteristic
of PVA/PANI hydrogel, PANI was used as a rigid polymer to enhance
either the antifouling performance of the platform or the conductivity.
Obviously, gelation of PVA as a soft polymer was caused by boric acid
groups on PANI yielding a hydrophilic and electrical neutrality plat­
form. Benefiting from double aptamers sandwich structure, aptasensor
probes have been designed for amplification of signal and sensitivity. In
this pursuit, the solution of thrombin signal aptamer and activated
magnetic NPs was incubated on PVA/PANI modified electrode
(Fig. 13A). The results indicated a satisfying high selectivity and sensi­
tivity with a LOD of 0.64 pM and linearity in the range of 1 pM-10 nM for
the determination of thrombin in real serum samples which reveals
potential application in clinical diagnostics and bioanalysis. Another
group [139] simply designed a new platform based on borax-reduced
AuNPs/PVA/thiolated aptamer for the determination of thrombin. The
designed platform exhibited specific and sensitive determination of
thrombin protein with a linearity range of 0.70 pM-0.02 mM. Comparing
the morphology characterization of PANI and the corresponding
hydrogel with the bare electrode in Fig. 13B revealed the successful
deposition of PANI and hydrogel on the electrode. Moreover, the anti­
fouling performance was evaluated using fluorescent microscopy as
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illustrated in Fig. 13C. This study gathered the advantages of aptamers,
NPs, and hydrogels which are favorable in sensing applications. To
broaden the wide application of PVA-based aptasensor with structural
similarity to the biological matrix, different aptamers could be labeled
on the AuNPs surface for detection of other analytes.
Generally, recent advances on aptamer functionalized DNA hydrogel
have explored their applications in clinical trials with the concerted
efforts of the researchers on their approval, quality control, effective
treatment, and design process. Although enormous efforts have been
made toward the applications of DNA hydrogels functionalized with
aptamer, there are still some challenges to be noted. The first one is the
lack of specific aptamers for their corresponding targets and their high
costs that limit the selection of effective methods for the construction of
aptamer/hydrogels. The lack of pharmacokinetic studies on aptamer
functionalized DNA hydrogel, which is essential for corresponding
guidance of rational applications, is the second challenge that limits the
rational design of hydrogel. The investigation of mechanical properties
is the other one that is significant in damage repair and artificial cell
construction.
2.7. Polymer nanomaterials/PVA hydrogel nanocomposites
Seminal efforts have focused on the concept of polymeric nano­
materials including homo/co-polymers, polymeric structures with
planned construction, formulated materials, and molecular shape
recognition materials in the sensitive sensors and biosensors field
[140,141]. Polymeric nanomaterials deliver a desirable application in
the biomedical endowed with distinctive properties [142–144]. A series
of polymeric NPs including conductive polymer (CP), dendrimers, li­
posomes, micelles, core-shell NPs, and nano-gels have been mostly
exploited in sensors due to ease of manufacturability, selectivity, line­
arity, and sensitivity [145,146]. By tuning bio-functionalization, dura­
bility, and signal transduction, the sensing performance of the polymer
NPs-based sensors could be enhanced [147]. By highlighting the
Z. Karimzadeh et al. Advances in Colloid and Interface Science 305 (2022) 102705

Fig. 12. schematic synthesizing of NiO/PVA/GQDs nanocomposite film using a solution casting process (A). Iso-surface maps for the intermolecular interaction
between PVA, NiO and GQD in two different configurations (B, C). Reproduced with permission from [130].

essential successes in the design of sensor platforms, the amalgamation
of the nanofiller and matrix contributions is pronounced to further
improvement [148]. Their integration into hydrogels via covalent or
non-covalent interactions imparts multi-functionality into the nano­
composite system because of multiple functional groups on the poly­
meric NPs [149].
Cellulose nanocrystals (CNCs) are insulating materials and a low-
weight binder, commonly used with conductive materials to construct
flexible substrates [150]. Abundant -OH groups on the surface of CNCs
induce their feasible surface functionalization and design novel
platforms with good foldability and flexibility [151,152]. Based on this,
Liu et al. [153] investigated wearable electronic sensors based on
conductive composite hydrogel by combining the tannic acid decorated
CNCs, rGO, and homogeneous PVA network. Briefly, CNCs were deco­
rated with catechol groups of tannic acid to enhance the mechanical
performances of the hydrogel. According to Fig. 14A, B, hydrogen bonds
and reversible dynamic borate bonds in the construction of the 3D hi­
erarchical structure inside the hydrogel impart the platform with elec­
trical and mechanical self-healing, robust and self-adhesive capability.
Furthermore, the formation of hydrogen bonds between oxygen groups

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Z. Karimzadeh et al. Advances in Colloid and Interface Science 305 (2022) 102705

Fig. 13. A) working principle of antifouling electrochemical aptasensor. B) SEM image of bare electrode (a), PANI/electrode (b), and nanocomposite hydrogel/
electrode (c). C) Representative fluorescence microscopy after incubation in fluoresceinisothiocyanate labeled bovine serum albumin (FITC-BSA) solution for 2 h.
Reproduced with permission from [138].

of rGO with the PVA network brings about the hydrogel with electrical
conductivity and mechanical strength as shown in Fig. 14C. Notably,
these mechanical and conductive behaviors were essential for real-time
and precise healthcare recording. The obtained platform holds prom­
ising applications in the detection of both large (e.g. joint bending) and
subtle (e.g. voice detection) human motions by variation of resistance
changes.
Besides, an artificial skin-like soft hydrogel has been developed
based on tannic acid-coated CNCs/AgNPs and PVA hydrogels by Lin
et al. [154]. Herein, CNCs extracted from bleached bamboo pulp were
consistently dispersed in the aqueous solution. The abundant catechol
functional groups on tannic acid-coated CNCs not only absorbed Ag+
ions via chelation but also accelerate the formation of AgNPs via its high
reduction capacity resulting in a color change of suspension (Fig. 15A).
The incorporation of Ag/tannic acid/CNCs into the PVA 3D network
hydrogel via dynamic borate ester bond cross-linking provides efficient
conductivity and super stretchability over 4000% (Fig. 15B). The dy­
namic borate ester bonds including didiol-borate bonds and catechol-
borate bonds, chain entanglement of PVA and Ag/tannic acid/CNCs
nanohybrids, along with the intra- and inter-molecular H-bonds syner­
gistically able the PB-Ag/TA@CNC hydrogels with an incorporated 3D
network (Fig. 15C and D). In the aqueous solution, borax easily disso­
ciated into tetrahedral borate ions and boric acid which could experi­
ence swift interchange between these two species as shown in Fig. 15E.
To sum up, the proposed platform demonstrated great potential in
constructing switches, repairing circuits, and electronic skin to monitor

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Z. Karimzadeh et al. Advances in Colloid and Interface Science 305 (2022) 102705

Fig. 14. Schematic illustration of the fabrication process for the A)TA@CNC, B) PB-TA@CNC-pRGO nanocomposite hydrogels, and C) the chemical structures inside
the hydrogel. (D) SEM image of the PB-TA@CNC-pRGO4 hydrogel. Reproduced with permission from [153].

human body motions through its facilitated electrons movements.
2.7.1. Conducting polymers
Among polymer NPs, conducting polymers (CPs) have been proved
an encouraging impact on the fabrication of conductive hydrogels to be
used in biosensing, chemical sensing, gas sensing, etc. thanks to their
unique electronic properties [155]. The concept of CPs includes poly-
3,4-ethylene dioxythiophene (PEDOT), PANI, polypyrrole (PPy) [156],
polyacetylene (PA), and polythiophene (PTP) which are π-conjugated
polymers with alternating single and double covalent bonds for con­
ducting electrons [157]. The associated delocalized π-bonding and
conjugated backbone structure define the characteristics of CPs [158].
The intrinsic conduction mechanism is caused by electron movement
along with the sp2-hybridized conjugation. The inclusion of CP moieties
into hydrogels has received considerable attraction recently because of
their tunable 3D matrix, swelling disposition, adjustable mechanical
properties, and high conduction. Two approaches have generally been
established for preparing CP-based hydrogels: First, aromatic monomers
are polymerized in insulating polymer solution as physical frameworks
which make the hydrogels with weak electrochemical activities and low
electrical conductivities [159]. Second, the CP chain is polymerized
along with the cross-linking process by adding cross-linkers. For bulk
scale, conductivity can occur by intramolecular hopping of adjacent
polymer chains via charge carriers which enhances the compatibility
between CPs and hydrogel network [160]. At this state, enormous efforts
have been made in investigating the biocompatibility of PEDOT and

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Z. Karimzadeh et al. Advances in Colloid and Interface Science 305 (2022) 102705

Fig. 15. Chemical structures of TA and CNC and schematic mechanism of TA@CNCs formation and AgNPs incorporation (A); Formation of nanocomposite hydrogel
(B); The possible chemical cross-linking reaction within hydrogels (C); SEM image of nanocomposite hydrogel (D); Multicomplexation between borax PVA and Ag/
TA@CNC (E). Reproduced with permission from [154].

PANI as two important polymers [161,162].
2.7.2. PANI
PANI is one of the greatest and most important CPs that harbors its
application in a number of sensing and biosensing systems. Cross-linking
of PANI with soft molecular chains by molecular interaction combines
the conducting paths of PANI with the mechanical merits of soft polymer
chains for the preparation of multicomponent or bicomponent hydrogels
[163,164]. In light of improving the elongation at the break of the PANI,
hydrogen bonding interaction plays a prominent role. PVA possessing
-OH groups are typically accepted as soft molecular chains for the cor­
poration with PANI [165]. Benefitting from that, Hu et al. [166] pro­
posed a facile approach for the preparation of self-healing and
stretchable PANI composite gel with superior mechanical properties. In
their rational design, polyacrylic acid (PAA) and PVA were used as soft
chains in PANI gel. Intended for providing multiple hydrogen-bonding
networks between materials, phytic acid with P=O/P-O groups were
employed in gel composite. Not only can -OH groups of PVA or -COOH of
PAA interact with P=O/P-O groups of phytic acid but also can -NH of
PANI. Therefore, the mechanical performance of rigid PANI is

19
Z. Karimzadeh et al.
impressively enhanced by the physical cross-link of hydrogen bonds
with PVA or PAA in the composite gel. Additionally, the extraordinary
performance of self-healing (around 100%) and stretchability were
assessed for PANI/PVA/PAA composite gel application in strain sensors.
All in all, this meaningful and practical insight explored its application
toward flexible sensors and energy storage devices. To broaden its wide
investigation, Wang et al. [167] synthesized PANI/PVA solution-
processable hybrid hydrogels for sensory electronic skins. The PANI/
PVA hybrid hydrogels were constructed by an oxidation procedure fol­
lowed by a cyclic freeze-thaw process. During the freeze-thaw process,
cross-linking was occurred by ionic interactions and crystal domains
generated. On account of the entirely physically cross-linked construc­
tion, the hydrogels in sensory electronic skins were completely regen­
erating and solution-processable. In this study, PANI and PVA were
selected as conductive and flexible components, individually. Further
enhancement in the flexibility of the PANI/PVA hybrid hydrogel was
obtained using water-glycerol binary solvents. Based on the results, the
flexibility and sensing ability was well retained at least for 7 days at
room temperature. Also, the elastic modulus of the hybrid hydrogels was
regulated from range of 15.7 to 154.4 kPa by tuning the PANI/PVA
contents. Additional studies revealed high stability up to 41000 cycles,
great sensitivity with GF of 4.28, excellent recyclability, and fast
response speed (250 ms). Hence, the proposed platform exhibit reliable
results for sensing representative human movements like joint bending.
2.7.3. PEDOT
PEDOT with a similar heterocyclic structure has drawn massive
consideration due to its high conductivity, small energy gap, and simple
molecular structure. The electron-rich oxyethylene of PEDOT leading to
lower reduction potential is considerably more stable. Nonetheless, the
low solubility and difficult dispersibility of PEDOT in water limit its
practical application. To improve the solubility in water, dopants such as
water-soluble polymer electrolyte polystyrene sulfonic acid (PSS) are
often used as a charge balancing dopant during the PEDOT polymeri­
zation process [168]. However, the most intractable limitation for pure
PEDOT: PSS is the low electrical conductivity and mechanical proper­
ties, impeding their widespread applications. To solve the problems of
PEDOT: PSS-based hydrogel, they either blend with other polymers
including PVA to create stretchably and conducting systems or are used
Fig. 16. Fabrication process of the SIPN PVA/PEDOT:PSS hydrogel (A); flexibility (B), stretchability (C), bendability (D) and electro-conductivity (E) properties of
the obtained hydrogels. Reproduced with permission from [173].
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Advances in Colloid and Interface Science 305 (2022) 102705
with polar solvents as secondary dopants to weaken the coulombic
interaction between PSS and PEDOT and facilitate the electron trans­
porting of PEDOT [168–170]. Lots of biosensors and strain sensors based
on PEDOT/PVA hydrogel have been successfully investigated owing to
the properties of the two polymer networks, mainly hydrogel distribu­
tion and mesh size [171]. As a pioneering attempt, Gao et al. [172]
prepared a flexible PEDOT: PSS/PVA hydrogel via a wet-spinning
method as a potential platform in wearable sensors. Herein, the
electro-conductive, mechanical and structural properties of PEDOT: PSS
were induced by the introduction of water-soluble PVA with high
modulus and EG treatment. PEDOT: PSS/EG/PVA hydrogel exhibited an
enhanced tensile strength of 210±5 MPa and breaking elongation of 26
± 1.5 % compared with pristine PEDOT: PSS fibers. Within the strain of
20%, a respectable durability and recovery performance of electro­
conductivity and the strain have been obtained for the proposed
hydrogel. Benefiting from all these advantages, it is indicated that this
composite conductive hydrogel not only improves the spinnability but
also endows it with more excellent applicability in functional textiles
and flexible sensors. More in deep, Zhang et al. [173] designed
conductive, stretchable, and flexible PEDOT: PSS/PVA hydrogel by a
facile two-step strategy as illustrated in Fig. 16. In this study, PEDOT:
PSS conductive chains were penetrated in the PVA network through
simple mixing and cross-linking with glutaraldehyde. The chemical in­
teractions and cross-linking network between PEDOT: PSS and PVA in
hydrogel matrix endowed them with excellent compression and tensile
properties for large-scale production. The designed PEDOT: PSS/PVA
composite hydrogel exhibited that the swelling ratio of hydrogels was
reduced by increasing the PEDOT: PSS content meantime, the electrical
conductivity of the hydrogels increased. According to the results, the
tensile strength of 70 KPa, elongation at breakage of 239%, and GF up to
4.4 (strain: 100%) were obtained for the composite hydrogels with 0.14
wt.% PEDOT: PSS. Inspired by all these attractive features, the designed
PEDOT: PSS/PVA composite hydrogel demonstrate great potential for
applications in wearable devices.
Substantial progress has been made in preparing PEDOT/PVA
hydrogels to develop electrodes for collecting the bioelectrical signals
using electrocardiogram (ECG) sensing technologies because of their
satisfying elasticity, toughness, and conductivity [174]. Inspired by the
water-rich content of the hydrogel electrode, not only can seamlessly
Z. Karimzadeh et al.
stick to the skin in the detection process but also promote the reception
of the ion current generated in the cells through the hydrating cuticle of
the skin epidermis. At this state, Wang and coworkers [175] fabricated a
flexible conductive electrode using PVA-based PEDOT: PSS/cellulose
hydrogel to monitor the ECG signals. For that, PEDOT: PSS was formed
in the process of oxidative polymerization of PVA and cellulose sub­
strates. The fibers with micron-level and linear at the beginning of
dissolution had a uniform thickness and was orderly arranged. Also, the
change in gel film from white to black during the oxidation process over
time has been observed. By controlling the PEDOT content, it has been
revealed that the conductivity of the composite hydrogel could be
accurately optimized. Also, no skin irritation was detected during the
signal measurement. This strategy could promisingly explore the
application of PEDOT: PSS/cellulose/PVA film in constructing eco-
friendly conductive electrodes for ECG monitoring due to admirable
features of stability, comfortable contact with skin, low skin contact
impedance, and flexibility.
3. Conclusions and outlook
Recently, the progress of nanocomposite hydrogel as an effective
nano-platforms for monitoring human motion and electronic skin has
witnessed excessive advancement. Herein, we aim to offer a compre­
hensive review discussing concepts and current progress in the devel­
opment of PVA nanocomposite hydrogel-based sensors, involving design
strategies, preparation approaches, and their applications. PVA nano­
composite hydrogels are emerging newfangled materials that possess the
properties of both soft matter gel and nanomaterials. Hence, a number of
studies comprising synthesis and physicochemical were pursued. The
microporous and hydrophilic building of the PVA hydrogels appears to
be an incredible host for NPs. In this context, the recent trends in
incorporating inorganic NPs, like carbon-based, LMs, 2D materials,
metal/MO, and polymer-based nanomaterials, into 3D polymeric net­
works as nanocomposite gels with appropriate functionalities for
adaptation to complex environments, are discussed. We specially out­
lined those PVA/NPs nanoprobes that are capable of identification in
complex media or those using novel constructions/approaches. As more
materials are advanced toward realizing particular characteristics and
buildings, PVA/NPs based hydrogel would attract further intensive
notice as functional nanoprobes. PVA-based nanoprobes with high me­
chanical characteristics have facilitated the construction of (bio)sensors,
flexible electronic devices, and biomedicine fields, which in turn their
performance relies considerably on the type and content of the NPs.
Particularly, the high conductive feature of this nanostructure permits
them to use in (bio)sensors, actuators, supercapacitors, electro-skin, and
drug delivers. Although various inspiring results were recently described
for PVA/NPs based hydrogel to realize high conductivity and stretch­
ability, their use often involves the phenomenon of agglomeration,
which requires more studies for precise control and development as a
comprehensive technique. In addition, the relatively poor interfacial
interactions between the NPs and polymers considerably induced the
low structural stability and mechanical features of the hydrogels. So,
exploring the NPs surface modification remains an imperative method to
improve their interfacial interaction with polymer via well-designed
bonding and structure. Additionally, the industrial-scale fabrication of
the nanocomposite is still challenging.
Nowadays, progress in processing approaches, for example, micro­
fluidic reactors, 3D printing technologies, dynamic cross-linking spin­
ning, and extrusion, afford extensive chances to advance large-scale
PVA/NPs based hydrogel with designed configurations. In this
perspective, PVA/NPs based hydrogel can be incorporated with 3D
printing as a molding fabricating strategy that can facilitate their
fabrication and effective implementations in different device applica­
tions. However, no significant progress has yet been made on the
printing of PVA nanocomposite hydrogels. The main reason is that 3D
printing technologies have a high demand for material performance,
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Advances in Colloid and Interface Science 305 (2022) 102705
such as the viscosity/melting point of the material, the photocurable
material features, and their capability to maintain the shape after
extrusion. To sum up, we believe that with the continued improvement
of procedures from the design to production of PVA/NPs based hydro­
gel, novel kinds of these hydrogels with arranged buildings, new re­
sponses to stimuli, and brilliant mechanical characteristics can come
true in the near future for use in the fields of (bio)sensors, actuators,
biomedicine, and biomimetic materials.
Declaration of Competing Interest
The authors declare no conflict of interest.
Acknowledgements
This report is a part of Z. Karimzadeh’s Ph.D. thesis submitted to the
Faculty of Pharmacy, Tabriz University of Medical Sciences, Tabriz,
Iran. The work is financially supported by the Pharmaceutical Analysis
Research Center under grant number of 68133.
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