Graphene Wearables

Chemical Engineering Journal 464 (2023) 142576
Contents lists available at ScienceDirect
Chemical Engineering Journal

journal homepage: www.elsevier.com/locate/cej
Review
Advances in graphene-based flexible and wearable strain sensors

Hui Chen a, Fengling Zhuo a, Jian Zhou a, *, Ying Liu a, Jinbo Zhang a, Shurong Dong b,
Xuqing Liu c, Ahmed Elmarakbi d, Huigao Duan a, Yongqing Fu d
a
College of Mechanical and Vehicle Engineering, Hunan University, Changsha 410082, China
b
College of Information Science and Electronic Engineering, Zhejiang University, Hangzhou 310027, China
c
Department of Materials, The University of Manchester. M13 9PL, United Kingdom
d
Faculty of Engineering and Environment, Northumbria University, Newcastle upon Tyne NE1 8ST, United Kingdom
A R T I C L E I N F O A B S T R A C T
Keywords: Flexible and wearable electronics have recently gained considerable research interest due to their potential
Graphene applications in personal healthcare, electronic skins, and human–machine interfaces. In particular, strain sensors
Stretchable that can efficiently transmit external stimuli into electrical signals are essential for wearable electronics. Two-
Strain sensors
dimensional carbon-based materials such as graphene are potentially versatile platforms for the above appli
Flexible and wearable electronics
cations, mainly attributed to their combined properties of excellent flexibility, thermal and electrical conduc
tivity, and mechanical strength. Although there are numerous reports devoted to the design, fabrication and
application of graphene-based strain sensors, a comprehensive overview dedicated on attributes of graphene-
based strain sensors that can be systematically correlated with their mechanisms, fabrication strategies and
applications is urgently required in the field. Specially this review is aimed to explore the following topics, i.e., (i)
the strain sensing mechanisms and key performance parameters of graphene-based sensors; (ii) the recent
progress of major graphene-based sensors including those of film-based, fiber-based, foam-based and hydrogel-
based; (iii) applications of graphene-based sensors for human motion sensing, health indicators, electronic skins
and human machine interfaces; and finally (iv) challenges and future directions for the design of graphene-based
sensors.
1. Introduction developing such wearable strain sensors include incorporating con

ducting components (e.g., carbon materials,[18] metal nanomaterials,
A vast range of applications, including personalized healthcare [19] and conductive polymers[20]) into the stretchable substrate, e.g.,
monitoring,[1-3] electronic-skin,[4,5] human–machine interfaces and polydimethylsiloxane (PDMS),[21] Ecoflex,[22] polyetherimide (PEI)
soft robotics,[6-9] etc., are being explored using flexible and wearable [23] and polyurethane(PU)[24]), or directly using electron/ion-
electronics. In these devices, external stimuli such as strain,[10,11] conductive hydrogels.[25].
pressure,[12,13] temperature,[14,15] humidity,[16,17] or various Graphene, one of the key 2D carbon-based nanomaterials well
deformation can be converted into detectable electronic signals (such as known for their superior electronic and mechanical properties, show
resistance, voltage, current, or capacitance). Among these, flexible great promises in numerous fields such as conducting wires, energy
strain sensors with high sensitivity, fast signal response, low storage and conversion devices, actuators, and catalysis.[26-31]
manufacturing cost, and reliable stability are good candidates for next Currently graphene and related materials have been demonstrated for
generation electronics in various wearable applications. For example, usages of electro-mechanical sensors with their high strain sensitivities
one can employ these devices on human skins for real-time human because of their good mechanical properties and also their dramatic
motion sensing. Conventional sensors made of organic and silicon ma changes of interlayer distances in responses to external strains. When
terials often suffer from critical problems when applied in such flexible synthesized and integrated into the matrix of composites, not only the
or stretchable sensory systems, including small strain sensing range, properties of the composites are enhanced, but also novel functionalities
non-linearity, and non-reversibility. Commonly used strategies for are generated for diverse uses. The distinctive properties of these
* Corresponding author.
E-mail address: [email protected] (J. Zhou).
https://doi.org/10.1016/j.cej.2023.142576
Received 17 November 2022; Received in revised form 25 February 2023; Accepted 21 March 2023
Available online 22 March 2023
1385-8947/© 2023 Elsevier B.V. All rights reserved.
H. Chen et al. Chemical Engineering Journal 464 (2023) 142576
graphene-based sensors are originated from the inherent characteristics and their key sensing performance parameters (e.g., sensitivity,
of the graphene, the combined functionalities of both graphene and stretchability). We then review recent progress regarding to the design
other elements in the substrate, or the synergistic effect between these and fabrication strategies of four major types of graphene-based strain
two. Moreover, other graphene derivatives such as graphene oxide (GO) sensors, including film-based, fiber-based, foam-based, and hydrogel-
and reduced graphene oxide (rGO) are easily obtained, further widening based ones. The following section provides an overview of graphene-
their scope of applications.[32,33] Research on graphene-based flexible based stretchable strain sensors for applications in human motion
sensors has become a highly exciting field as publications have increased sensing, health indicators, electronic skins and human–machine in
exponentially over the past two years. Despite of this, graphene and its terfaces, etc. Finally, key challenges and future perspectives in the
related materials remain a great challenge for sensing applications, promising fields of wearable electronics using the graphene and related
especially for graphene-based flexible or wearable sensors. materials are discussed.
Recently, several reviews have been published on the development
of flexible and wearable electronic sensors using graphene and related 2. Strain sensing mechanisms and performance
materials, or other carbon materials such as graphite and carbon
nanotubes (CNT).[34-37] Nevertheless, these reviews are primarily 2.1. Strain sensing mechanisms
focused on the development of general carbon-based materials for
wearable sensors,[18,38] flexible conductive electrodes,[39,40] and Depending on the fabrication processes, micro/nanostructures, and
energy devices.[41,42] For example, Wang et al. [43] published a sensing materials, graphene-based flexible strain sensors have various
comprehensive overview of different types of carbon-based flexible strain response mechanisms. For example, the sensing mechanisms of
electronics and their applications. Yan et al. [44]summarized advances conventional resistive strain sensors are mainly originated from the
in 2D materials based wearable electronics for monitoring human geometrical effect and the piezoresistive effect of the materials, whereas
physical and chemical signals. However, a detailed overview of recent some new sensing mechanisms such as disconnections among sensing
progress in graphene-based flexible and stretchable strain sensors, elements, crack propagation in films, and tunneling effect are frequently
especially their design methods and applications, has not been reported used to tune the electromechanical responses of stretchable strain
as far as we have searched. sensors.
This review will provide a full spectrum of specific and potential
topics of graphene-based stretchable strain sensors, especially for their 2.1.1. Geometrical effect
key mechanisms, design methodologies and major applications. In this The geometrical effect of the resistive-type strain sensor means that
review, we firstly introduce the working principles (e.g., geometrical upon stretching, the sensing and conductive material is stretched, but it
effect, piezoresistive effect) of graphene-based flexible strain sensors is contracted in the transverse direction of the stretching direction in
Fig. 1. Sensing mechanisms of stretchable graphene-based strain sensors. a) Geometrical effect. b) Piezoresistive effect. c) Disconnection mechanism. Reproduced
with permission [58]. Copyright 2022, Springer Nature. d) Crack mechanism. Reproduced with permission [65]. Copyright 2019, Elsevier. e) Tunneling effect.
2
light of its Poisson’s ratio ν. Therefore, it will cause the changes in reduce the resistances of the composite. Some graphene flakes tend to
lengths or cross-sectional areas of the conductive material, and its slip, shift or move at a low strain (e.g., below 125%). Nonetheless, they
resistance will be changed (Fig. 1a). This geometrical effect of the are still in good contact with each other, and the percolation pathways
resistance follows the formula below: remain effective, hence the strain sensor has a GF value of about 21,
which is extremely low for small strain sensors. Evidently, by applying
L
R=ρ larger strains (300%), graphene sheets become not only significantly
A
separated but also change their stacking patterns, accompanied by the
where ρ denotes the resistivity of the material, L represents the length, appearance of ridges, which reduces conductive channels and remark
and A is the cross-sectional area of the material. As the resistivity of the ably increases the sensitivity to 191. Finally, the GF value of the sensor
sensing material is normally a constant, the resistance will be increased reaches a peak of 1087 at 600%.
with the stretching of the sensing material and shrinking along its cross-
sectional direction. Many metal-film based flexible resistive strain sen 2.1.4. Crack propagation
sors employ their dimensional changes as the response mechanisms, and When brittle thin films which are coated on polymers are under
they have been extensively applied due to their straightforward pro stretching, cracks can be generated and propagate due to the mechanical
duction techniques and simple structures.[45,46] Moreover, Wang et al. mismatch between these two materials. As microcracks are gradually
[47] employed 3D printing technology to produce controllable micro open and enlarged, the conductive paths are drastically reduced,
structures in graphene/PDMS strain sensors. Based on the geometrical resulting in a drastic increase in electrical resistance. In fact, cracks,
effect, the gauge factors for hexagonal, triangular, and grid composite which can release external stress, are prone to occur in the locally stress
structures were predicted. Similarly, Vu et al.[48] used the geometrical concentrated areas. In spite of the fact that cracks are normally unfa
effect to inversely derive the resistivity of a strain sensor fabricated from vorable in structural designs, formation of microcracks can be an
the mixture of silver paste and single-walled carbon nanotube. effective way to enhance sensing performance, sometimes in conjunc
tion with other mechanisms (e.g., disconnection mechanisms), thus
2.1.2. Piezoresistive effect becoming an effective approach for strain sensors.[59-62].
A piezoresistive effect occurs when structural stress or strain changes Generation of micron-scale cracks has often been observed in
a material’s resistivity, and the resistance change can be expressed as graphene-based thin films coated on soft polymers under the external
follows: force.[63,64] For instance, Yang et al.[65] explored the morphological
evolution of layered strain sensors based on Ti3C2Tx /graphene/PDMS
ΔR Δρ
= (1 + 2ν) + under different strain states (0–70%), as shown in Fig. 1d. As the com
R ρ posite film was unstretched, it had no apparent cracks and was closely
The term of 1 +2ν indicates the influence of geometrical changes (i. packed with fine Ti3C2Tx particles and graphene sheets. When 10%
e., geometrical effect), while the latter one of Δρρ expresses the piezor strain was applied, the stacking density of nanomaterials was not
changed notably. However, a few small cracks were emerged perpen
esistive effect of the material itself (Fig. 1b). For metals and metal-alloy
dicular to the tensile direction on Ti3C2Tx /graphene upper layer, indi
materials, their resistances are commonly increased by a few times.
cating that the tensile stress was released through formation of these
Despite this, for semiconductors materials such as germanium and sili
cracks. Graphene/PDMS bottom conductive layer was gradually
con, their resistance changes can be multiplied by a considerable factor
exposed as the cracks are expanded from 1 μm to over 3 μm under 30%
due to the changes in their bandgaps or inter-atomic spacing, thus
strain. In the presence of 70% strain, the cracks continuously grew,
achieving high performance.[49-51] In spite of considerable efforts to
followed by local rupture of the bottom layer, as well as graphene
bolster the functionality of these piezoresistive strain sensors, flexible
slippage, leading to a high sensitivity.
strain sensors are capable of measuring strains far beyond the limitations
of those conventional electronic devices (ε < 5%).[52,53] Moreover, the
2.1.5. Tunneling effect
piezoresistive sensors often showed poor responses under high dy
The phenomenon describing the transmissions of electrons through a
namic/frequency conditions due to their limited response times, which
non-conducting barrier is called tunneling effect, and it is a crucial
is tens of microseconds.[54] To overcome these shortcomings, several
quantum effect in physics. Furthermore, electrons can completely
methods have been developed to overcome these shortcomings by
transmitted (or tunneling) through closely spaced adjacent nano
combining composites of nanomaterials and elastomer matrix to form
materials.[19,66] Within a definite cut-off gap between adjacent nano
strain sensors with superior performance.
materials, electrons can pass through a thin polymer layer and create a
quantum tunneling junction. The tunneling resistance between two
2.1.3. Disconnection mechanism
neighboring nanomaterials can be approximated according to the Sim
The disconnection mechanism mainly exists in the conductive net
mon’s principle: [19]
works such as those with graphene flakes, in which electrons are able to
( )
pass through freely overlapped nanomaterials. When the conductive V h2 d 4πd √̅̅̅̅̅̅̅̅̅
film is subjected to an external strain, some of the interconnected Rtunnel = = √̅̅̅̅̅̅̅̅̅ exp 2mλ
AJ Ae2 2mλ h
nanomaterials are stretched and separated, thus reducing their over
lapped areas and electrical connections, and increasing their electrical where V denotes the electrical potential difference, A is the cross-
resistances. Vice versa, when the strain is released, those nano-stacks are sectional area of the tunneling junction, J is the tunneling current den
reconnected and the conductive contacts are recovered, thus their sity, e is the single electron charge, m is the mass of electron, λ is the
electrical resistances are restored. As seen from a microstructural height of energy barrier for polymers, h is Plank’s constant, and d is the
perspective, the weak bonding and stiffness mismatch between the distance between adjacent nanomaterials. The cut-off distance depends
nanomaterials and elastomer are responsible for nanomaterial’s slip on several factors, namely, matrix material, processing parameters, and
page effect.[19,55]. conductive fillers.[67] For example, the maximum tunneling distance in
Strain sensors based on flakes and sheets exploit this mechanism of CNT-based polymeric composites was reported to be ~ 1.8 nm,[66,68]
disconnection.[52,53,56,57] For example, Zhou et al.[58] investigated whereas that for two parallel graphene sheets insulated with polymers
the morphological evolution of graphene/Ecoflex composites at various was ~ 2–3 nm.[69,70]
stretching states (0–600%), as shown in Fig. 1c. Before stretching, gra Using graphene-based materials as an example, the conductive net
phene flakes are self-overlapped and form a conductive network to works show relatively compact graphene sheets in their original state
3
(Fig. 1e). When stretched, the graphene sheets are unfolded with the where R0 and R are the resistances without and with applying the strain,
polymer matrices chains, causing an increase in the tunneling distance respectively, and ε is the applied strain. The GF values of stretchable
between the sheets, which results in the destruction of the conductive strain sensors are related to many factors, including conductive mate
pathways and the increased resistance. The tunneling effect often causes rials, microstructures and preparation processes.[76,77] Previous
an exponential increase in electrical resistance. Previously, it has been studies have shown that the conductive layer plays a dominant role in
demonstrated that graphene-based strain sensors can achieve a high the sensitivity of the sensor, and the tunneling effect causes a greater
sensitivity (up to 600 at 2% strain) with the tunneling effect.[71-73]. increase in resistance than the other mechanisms.[74,78,79] An increase
In summary, the conduction mechanism mentioned above can be in sensitivity will improve the signal-to-noise ratio of the sensor, making
explained by the induced changes of resistance values caused by struc it desirable for most applications. The graphene hydrogel
tural deformation. Among these five mechanisms, the geometrical effect nanocomposite-based strain sensors show a relatively low GF of 1–15 in
and the piezoresistive effect are the conventional strain induced sensing tension,[80-82] while the film-based sensors can be structurally
mechanisms, which can be described using the equation R = ρ L/A. The designed to have a sensitivity>600 in a small range.[74,83-85]
former one (e.g., the geometrical effect) is due to the changes of Pois
son’s ratio of the material, resulting in the opposite changes in length 2.2.2. Stretchability
and cross-section during deformation. Whereas the latter one (e.g., the Stretchability refers to the maximum strain that the sensor remains
piezoresistive effect) is based on the resistivity changes of the material. intact, and it not only requires the sensor to withstand high tension, but
We should address that strain sensors based on these two mechanisms also requires the sensor to maintain stable mechanical and sensing
often suffer from large hysteresis and nonlinearity. performance under large strains. The stretchability is the primary
By combining nanomaterials and elastic matrix composites, several consideration for researchers when designing artificial skin, which is
new mechanisms, including disconnection among sensing elements, used on arbitrarily curved surfaces which are often repeatedly
propagation of cracks within the films, and tunneling effects, can deformed, such as robotic hands. Notably, a larger strain (e.g., >1000%)
effectively induce structural deformation of the conductive networks, may cause an inelastic stretching stage where the elastomer has trouble
thereby increasing the resistances of their corresponding strain sensors. recovering or even fails catastrophically. Therefore, a superior stretch
The disconnection mechanism is originated from a large stiffness ability does not guarantee the successful application in a broad working
mismatch between the nanomaterial and the stretchable substrate ma range of strains. The requirement for flexible sensors with high
terials, resulting the slippage of nanomaterials under a large tension. For stretchability is emerging, driven by a range of applications such as
the crack propagation mechanism, during stretching, cracks are often wearable healthcare devices, robotics, and electronic gloves utilized in
initiated and then propagate in the brittle film coated on the soft poly tele-surgical procedures.[86] A major challenge, however, lies in
mer layers. The tunneling effect mechanism is related to the quantum manufacturing strain sensors with both a large stretchability and supe
effect, and the resistance value of the sensor generally increases expo rior GF. Performing considerable structural deformation is essential for
nentially according to the Simon’s theory. Despite its similarity to the achieving a high sensitivity. Nevertheless, high stretchability requires
disconnection mechanism discussed above, the tunneling effect differs materials to keep morphological integrity or structural connection.
remarkedly from the later one due to its weak bonding and stiffness These two traits are difficult to accomplish through simple sensor
mismatch. structures.
To choose a suitably responsive mechanism, it is important to
investigate the deformation of the conductive network structure of the 2.2.3. Linearity
strain sensor during its deformation process. For example, an in-situ Linearity of a strain transducer is usually expressed by the coefficient
analysis using scanning electron microscope (SEM) can be done to of determination (R2) derived from a linear regression, by quantifying
observe the morphology changes of conductive materials (i.e., graphene ΔR/R0 versus the strain curve. A high-quality linear strain sensor should
nanosheets) on the sample surface in real time during the stretching have a larger R2 value with a negligible deviation from a straight line in
process. Displacement can be observed among the nanosheets for the the output signals. Generally speaking, once the microstructure of
disconnection mechanism, while in crack propagation dominated sensing materials is changed from a homogeneous morphology into a
graphene-based sensors, the density of cracks and their sizes are grad nonhomogeneous one (for example, due to the formation of cracks in
ually increased. For the tunneling mechanism, an exponential increase thin films made of graphene flakes[63,64,87]), the sensor’s responses
in the resistance value is usually observed during stretching, which is become nonlinear with the applied strain. A high linearity of the rela
caused by the increased distance between adjacent nanomaterials. tionship between external stimuli and electrical signals can avoid the
[74,75]. complicated calibrations for strain-response of sensors, thus simplifying
data processing and circuit design and increasing the response speeds.
2.2. Performance of stretchable strain sensors For most strain sensors, there is often a trade-off between excellent
sensitivity and high linearity, e.g., the linearity is usually sacrificed for
Different performance parameters can be used to evaluate stretch achieving a high sensitivity in graphene nanocomposite hydrogel-based
able strain sensor performance, including sensitivity (often represented sensors. Both of them can be improved by formation of uniform com
by the gauge factor), stretchability, linearity, hysteresis, response time, posite network structures through a rational design. For instance,
and durability, etc. These parameters mentioned above should be taken considering different sensing mechanisms simultaneously, a graphene
into account while designing stretchable strain sensors, including those nanocomposite–based strain sensor, which was made through one-step
of graphene-based ones. screen-printing method, demonstrated an outstanding sensitivity (GF
> 400) and four linear regions with an R2 value exceeding 0.98.[85].
2.2.1. Sensitivity or gauge factor (GF) The linear responses for these sensors are attributed to the homogeneous
Strain sensitivity of the sensor is usually expressed by the GF (where crack formation, and this phenomenon was frequently observed in strain
higher GF levels imply higher sensitivities), which can be calculated sensors made of brittle materials with uniform structure and limited
from the slope of the relative resistance change (ΔR/R0) versus the stretchability.[88,89] Moreover, it was reported that the generated
strain curve, i.e., cracks often exhibited different structures or morphologies under
different strain ranges, e.g., parallel linear microcracks at a 20% strain
GF =
ΔR/R0 and wavy structures at a 60% strain, which is the main reason for the
ε different linear regions of the sensing curves.[85].
4
2.2.4. Hysteresis the structures of graphene composite materials, they can be classified
Under the same test conditions, hysteresis of a sensor occurs when into four groups, e.g., (1) film-based strain sensor; (2) fiber-based strain
the loading and unloading curves do not coincide during tensile cycling. sensor; (3) foam-based strain sensor; and (4) hydrogel-based strain
This effect is usually cumbersome and undesirable, but its correction can sensor. Both the designs of materials and structures are crucial for the
be achieved through signal processing and comprehensive character development of next-generation wearable graphene-based strain sen
ization of the sensor’s response. In skin-mountable or wearable appli sors. This section is mainly focused on the preparation methods, repre
cations, where strain sensors are operated under a dynamic loading sentative examples, advantages and disadvantages of each type of
condition, hysteresis becomes a critical consideration. In these cases, graphene-based strain sensors. The details of main features of each
significant hysteresis of the sensor results in its irreversible sensing graphene-based strain sensors are presented in Tables 1- 4.
properties under dynamic loadings.[90] The viscoelastic of polymeric
substrates and their interaction with nanomaterials (e.g., graphene or 3.1. Film-based strain sensors
CNT) result in large hysteresis in stretchable resistive strain sensors.
[19,68,91-93] A weak bond between the filler and matrix enables the Graphene and rGO films can be prepared using chemical vapor
filler to slide easily within the matrix during large stretching, which deposition (CVD),[108] dip coating,[83] spin coating,[109] spray
results in the hysteresis behavior since the filler takes a long time to coating,[110] vacuum filtration,[111] and wet- spinning.[112] The
return to its original position after releasing the strain. Hence, enhancing remarkable combination of impressive electrical conductivity and op
the interfacial binding between nanomaterials and polymers is an tical transparency in graphene films makes it an attractive material for
effective way to minimize hysteresis.[94-97] In contrast, a strong fabricating flexible sensors. A flexible and transparent PDMS composite
interfacial binding will often cause the nanomaterials to become buck has been reported through introduced chemically treated rGO into
ling and facture, or result in a poor stretchability.[19,98] A good hys elastic polymers as a filler.[113] Adjusting the rGO distribution uni
teresis performance in strain sensors will therefore require additional formly can achieve 82% transparency with such flexible matrix. As an
studies to optimize interfacial interactions, such as modifying active alternative to the above conventional methods, laser scribing can pro
groups.[96]. duce graphene with different patterns using carbon-rich precursors,
[102,105,114,115] although randomly distributed cracks and high
2.2.5. Response and recovery time temperature treatments caused problems such as poor sensitivity.
The time that it takes the sensor to alter its own output after an Microstructured conductive layers (e.g., scale-like,[73,116,117]
instantaneous change in its input is called response time, typically nanowall-like,[118] wave-like,[106] and wrinkle-like[104]) or elas
measured as the time to reach 90% of the measurement reading. Re tomer (e.g., PDMS[119]) have been demonstrated to improve film-based
covery time is the time for the sensor to return back to its steady state strain sensors’ sensitivity (Fig. 2a-c). As an example of the former case,
after the external force is removed. Both times will determine the an extremely thin graphene film (2.5–5.0 nm) engineered with fish
sensing speed of the strain sensor.[76,99] The magnitudes of the scale-like structure was found to be capable of achieving high sensitivity
response/recovery time directly determine the frequency that the strain (an GF value of 1037 under a strain of 2%) and showing a good trans
sensor can detect. The flexible strain sensors made of ultra-soft elasto parency (>86%), via a self-assembly method based on the well-known
mers often show a certain degree of response delay.[100] For example, Marangoni effect.[73] For the latter case, Yu et al. recently fabricated
vertical graphene nanosheets-PDMS strain sensors and laser-induced two-sided topological architecture (auxetic/sinusoid) flexible PDMS
graphene-Ecoflex elastomer composite strain sensors have the recov substrate, and demonstrated ultra-high sensitive (GF value of 1744 at a
ery times of about 960 and 70 ms, respectively.[101,102] For flexible train of 5%) rGO nanocomposite strain sensors.[119] Besides, several
strain sensors consisting of fillers and elastomers, potential frictions may types of rGO/PDMS sensors were also developed by altering the distri
lead to longer recovery times in the releasing cycle, which is evident in bution of the topographic designs (Fig. 2d). Furthermore, considerable
the case of graphene-based hydrogel sensors that require long recovery effort has been made to expand these sensors’ working strain ranges
times.[76,86,99]. while maintaining their superior sensitivity.[74,83,84] Shi et al.[85]
reported ternary nanomaterials of different dimensions-based strain
2.2.6. Dynamic durability sensors by integrating layer-slippage and crack-propagation mecha
Dynamic durability represents the endurance of the strain sensors nisms, exhibiting a sensitivity of 2392.2 with a wide-broad stretchability
over long stretch/release cycles. It provides stable electrical function (>50%) and was utilized for monitoring subtle strains of human body
and mechanical integrity. Durability is essential for skin-mountable and activities monitoring. In the nanocomposite film, due to its brittleness of
wearable strain sensors. This is because strain sensors should be certain components, cracks easily develop when stretched. However, 0D
accommodated through extremely large, complex and dynamic strains. fullerene (C60) reduces friction between graphene slides and accom
In the past, many researchers confirmed that the degradation of strain modates some of the applied stress, extending the working range and
sensor’s performance was mainly due to fatigue and plastic deformation maintaining high sensitivity.
of polymer substrates under high strain and fracture and buckling of A strain sensor is considered practical only if it can accurately and
sensing nanomaterials.[19,103] Nevertheless, it has also been claimed consistently detect the desired range of strains. Hence, cycling stability
that significant dynamic durability is often present in some stretchable should be considered when defining a sensing range. It has recently been
strain sensors as well. Highly durable and stretchable graphene-based revealed that strain sensors based on films are unstable over an extended
strain sensors have recently been reported to show remarkable dy period, as the cyclic stability is an important parameter for their prac
namic durability, e.g., up to 5000 stretching–releasing cycles.[104-107] tical applicability.[120-122] For instance, Qiao et al.[121] presented a
For example, high durability values of 5000 and 10,000 stretching/ strain sensor fabricated by laser scribing graphene (LSG) with an
releasing cycles have been reported for strain sensors made of the gra enhancement in the sensor’s sensitivity but with degradation during the
phene/PDMS and rGO/PDMS composites under strains of up to 50% and cyclic loading process (Fig. 2e). Zhang et al.[122] solved this problem in
10%, respectively.[84,104]. a pragmatic way by developing hybrid carbon filler sensors, i.e.,
combining carbon nanofibers (CNFs) and graphene nanoplates (GNPs),
3. Classification of graphene-based stretchable strain sensors obtaining a significantly better cyclic performance (1000 cycles from
0 to 50% strain) when compared to the equivalent sensors incorporating
A variety of graphene-based flexible/stretchable sensors have been only one filler (Fig. 2f). However, it should be addressed that the
developed by incorporating graphene or graphene derivatives (e.g., GO changing signals of the electrical resistances, which reflects the
and rGO) into the stretchable substrate for strain sensing. According to stretched strains, are commonly unstable during the initial stages of the
5
Table 1
Summary of main features of graphene film-based strain sensors.
Materials Method Stretchability Gauge factor Cyclic stability Response time Ref.
(ms)
PEI-rGO/PDMS Self assembly / 1744(5%) 6000(2%) / [119]

rGO/PDMS Vacuum filtration 300% 19.24(0–8%) 10000(10%) 90 [104]
170.70 (8–20%),
9156.29 (20–170%)
55 785.76(170–270%)
167 665.61 (270–300%)
graphene ink/PDMS Spray coating / 1054(26%) 500(13%) / [116]
UGF/PDMS Self assembly / 1037(2%) / / [73]
rGO Vacuum filtration 200% 16.2(0–50%) 5000(10%) / [117]
150(60%)
GNW/PDMS MPCVD / 5000 – 86,000 >800(3%) / [118]
(1 – 4%)
LIG/PDMS Laser / 150–2203.5(0–6.8%) 15000(5%) / [106]
AGNW/GO/C60 Screen-printing / 25(0–3%) 3000(40%) [85]
466.2(3–35%)
1000.2(35–52%)
2392.9(52%-62%)
graphene/PDMS LB assembly / 4304(93.3%) 3000(40%) 50 [83]
3D-GF-900/PDMS CVD 187% 1500(100%) 5000(50%) 50–81 [84]
CNF/GNPs/PDMS Spin coating / 5.15(0–47%) 1000(50%) 132 [127]
LPG/Ecoflex Laser / 160(35%) 180(25%) <20 [120]
LIG/Ag/PDMS Laser / 183(0-%8) 500(4%) / [122]
475(8–14.5%)
LSG Laser / 11(0–2.5%) 1000(2%) / [121]
92(2.5%-4.5%)
673(4.5–5%)
VGNs/PDMS PECVD ～120% 32.6(120%) 1000(20%) 960 [101]
VGA Dip coating / 6980(250%) 2000(20%) / [128]
graphene/KCL Drop casting 300% 25.2(294%) 1200(10%) 80 ms [129]
/Ecoflex
GMSN/PDMS Self-assembly 400% 0.37(10%-100%) 500(1%) / [130]
graphene/rubber Spray coating 25% 35(5%) 100(5%) / [131]
LIG/Ecoflex Laser / 1.68(0–6%) >1500(20%) 70 ms [102]
4.52(6–30%)
91.55(42–50%)
Graphene nanopaper/PDMS Vacuum filtration 100% 7.1(100%) / / [53]
G-putty/PDMS Screen-printing / 110 >1800(2%) / [132]
RGO/PDMS laser scribing / 23.4(0–2.5%) / / [133]
99.9(2.5–5%)
402.3(5–7.5%)
MDS-LIG/PDMS laser scribing / 236.2 (0–16.7) 12000(4%) 250 ms [105]
1242 (16.7–25)
tensile cycle, thus leading to an error-prone measurement of the strain. 3.2. Fiber-based strain sensors
Furthermore, although the resistive signals could eventually stabilized
after dozens of continuously stretching cycles, the unstable state of Human body motions can be easily captured with fiber-based sen
signals were manifested after testing in the following cycles.[123] Ac sors.[134] Additionally, fiber-based strain sensors can prevent large or
cording to several studies, graphene-based strain sensors often suffer even irreversible cracks from developing within a wide range of strains,
from cycling instability under the tensile cycles.[124-126] Qi et al. thereby preventing large or even irreversible damage.[135-138] Nor
proposed to improve the interactive forces among adjacent rGO sheets mally, graphene fiber-based strain sensors can be achieved using a
through introducing polydopamine and Ni2+, avoiding temporary spinning process and surface modifications, including blending active
sliding due to wrinkle graphene layer, which is a good solution to this materials or modifying surfaces of existing nonconductive fibers.
problem.[123] The obtained rGO/PDA/Ni strain sensor not only has a Through tweaking spinning factors such as conductive material density,
high cycling stability, but also a six-fold increase in sensitivity (Fig. 2g). spinning hole size, and speed, composite fibers can be designed with
In addition, in complex application scenarios, such as those with various conductivity, diameters, and shapes. For the spinning method,
perspiration, high relative humidity, or liquids, strain sensing capabil sensors are not easily capable of achieving both good mechanical and
ities can be significantly compromised or even totally destroyed. conductive properties. As one of the most efficient and useful methods
Treating the sensor’s surface with a superhydrophobic coating could be for the preparation of conductive fibers, surface modification can be
a potential method to solve the issues discussed above. In the presence of realized by covering materials on the surface of fiber. As a result of its
a superhydrophobic layer, water droplets may rebound quickly without conductive elements, the fiber has an excellent conductivity, however,
affecting the sensor’s performance. For instance, by utilizing rGO film poor washability could be an issue for real applications.
and VHB substrate as the raw materials, a wearable and waterproof
strain sensor was constructed by employing a biaxial pre-stretching 3.2.1. Spinning
method for wrinkle structure (Fig. 2h).[104] Such a sensor exhibited For the spinning methods, wet-spinning is an efficient method of
super-hydrophobicity and anti-corrosion property in light of the low fabricating fibers at large scales. Previously a coaxial wet-spinning
surface energy and high roughness of the layer (Fig. 2i). approach with post-treatment processes (Fig. 3a) was demonstrated to
prepare hybrid fibers with core–shell segmental configuration for strain
sensing.[139] A change in the extrusion speed can be used to adjust the
6
Table 2
Summary of main features of graphene fiber-based strain sensors.
Carbon materials Method Stretchability Gauge factor Cyclic stability Response time Ref.
FLG/SBS Wet-spinning 700% 160 (0–50%) / / [140]

2546 (50–100%)
Graphene/CNT/BCN/TPU Wet-spinning / 17.8 (0–70%) 10,000 (50%) ≈ 100 ms [107]
326.6 (70–150%)
1501 (50–230%)
Graphene/PVDF/PU Wet-spinning / 51 (0–5%) 6000 (1%) <100 ms [141]
87 (5–8%)
rGO/TPU Electrospinning 670 ± 20% 11(0–10%) 6000 (50%) 200 ms [146]
79(10–100%)
GNPs/CNC/ Electrospinning 897 ± 1% 75.1 ± 1 (0–10%) 2000 (10%) 100 ms [144]
Mxene/SBS 168.7 ± 5 (10–50%)
400 ± 7 (100–350%)
SiO2/graphene/PU Electrospinning 405.4% 1.1 (0.22%) 600 (50%) / [145]
3.0 (22.94%)
5.9 (94.110%)
MWNT-rGO@PEB Dip coating / 150 (0%–25%) 2000 (36%) 70 ms [155]
650 (28–40%)
rGO/SF Dip coating / − 8.89 (0–5%) 580 (0.3%) / [168]
16–0.7 (10–50%)
G@PVA fiber CVD 16% 5.02 (1–6.3%) 200 (6%) / [169]
Ag@rGO@PDMS Ultrasonication 210% 420(0–2%) 3500 (60%) 130 [170]
1.1 × 109(10–50%)
TGF Wet-fusing assembly 48.50% 63 (0–60%) 3000 (30%) 90 ms [171]
rGO/ANF/NR Ultrasonication >200% 22.6 (0–100%) 1000 (10%) 195 ms [172]
131 (100–158%)
363 (158–200%)
870 (200–226%)
Graphene/PU /PVA LBL 50% 86.86(0–50%) 100 (50%) / [163]
GNP/AgW/PU/PDA LBL 500% 139.6(00.01%) / / [159]
198.8(0.01–125%)
PU/GNS/Au/GNS LBL / 661.5 (0–50%) 10000(50%) 10 ms [161]
/PDMS
668.33 (50–75%)
PU/GMs//AgNPs LBL / 490.2(0–50%) 2000 (50%) / [166]
/PDMS
graphene/rubber/nylon/wool LBL RY:100% RY:1800 / / [160]
NCRY:150% NCRY:1.4
WY 50% WY − 0.1
Rubber/graphene Spray coating 310% 7.1 (0–200%) 1000 (50%) / [158]
53 (200–310%)
rGO/PE Spray coating / 6.4–12.6 / 91 ms [165]
CNT/rGO/PU Spray coating 1340% 38.1 (1–200%) 1000 (50%) / [173]
317.4 (200–350%)
781.4 (450–550%)
2160.4 (550–620%)
M-rGO@KH-EPY Dip coating 180% 576(0–50%) 5000 (50%) / [167]
862 (>50%)
FB/CB/GNPs Ultrasonication 60% 5.62 (0–4%) >1000 (8%) / [153]
PAN/graphene Electrospinning / 1700 (0–2%) 300 (2%) / [174]
thickness of the core and shell layers. In the example above, the thick
Table 3 ness of the shell/core layers was varied from 192/796 mm to 96/1010
Summary of main features of graphene foam-based strain sensors.
mm as the core flow rate was increased. Similarly, through wet-
Carbon Method Stretchability Gauge Cyclic Ref. spinning, a fiber-based strain sensor was developed by mixing poly
materials factor stability
(styrene-butadienestyrene) (SBS) and few layer graphene (FLG) with
GF/PDMS Self- 30% 98.66(5%) 200 [190] different weight percentages (Fig. 3b).[140] It was reported that the
assembly (20%) SBS/FLG fibers with a higher FLG loading showed a lower tensile
AgNWS@TGF/ Template 60% 11.8(60%) 800 [185]
FPU (25%)
strength and a lower elongation, mainly due to increased agglomeration
GF/SBR Template / 250(86%) 500 [184] and porosity as the sources for cracking. Similarly, composites with
(30%) graphene contents marginally over the critical value often form sparsely
GPN/PDMS CVD / 2.6 10(25%) [186] distributed conductive networks which are less conductive but more
(0–18%)
easily deformable, thus resulting in better sensitivity at the same level of
8.5
(22–40%) strain. In contrast, when the graphene content is substantially exceeding
FGF/PDMS CVD 70% 2.4–15 1000 [95] the threshold, the sensor usually exhibits its lower sensitivity due to the
(8.5–77%) (50%) dense conductive network. The strain sensor made of composited fibers
with 3 wt% FLG showed a high tensile strength of ~ 18.3 MPa, a
maximum failure strain of > 700% and a high sensitivity (with a GF of
2546 under a strain of 100%). Other types of composite fibers such as
graphene/CNT/bacterial cellulose nanofibers (BCN)/ thermoplastic
7
Table 4
Summary of main features of hydrogel-based strain sensors.
hydrogel Stretchability Gauge factor Cyclic Stability Response times Ref.
(ms)
Tensile strain Tensile strength
(kPa)
PAM/SF/GO/PEDOT:PSS (PSGP) 600% / 0.8(0–50%) 2000(50%) 170 ms [81]

1.6(50400%)
0.6(400%-600%)
PAA/CS/GO/Gly >1000% / 1.138(0–80%) 1000(20%) 40 ms [80]
4.7(>80%)
PVA/glycerol/CC/GO / / 1.06(0–175%) / / [203]
(PGCY) 1.9(175–300%)
PAA/PDA-rGO/Fe3+ >600% 400 1.32(100–500%) / / [214]
PVA/PC/rGO 5000% / 4.29 (0–60%) / / [217]
5.26 (60–260%)
14.14 (260–550%).
GA/rGO/PAM 2094% 118.7 2.496(0–40%) 150(150%) / [218]
3.957(40–100%)
15.467(100–1000%)
rGO/SA/PAM 312% 143.2 2.09(0–250%) 200(100%) 200 ms [212]
SC-PDA/GO/Ca2+/PAM (SPGCP) 10300% / 3.28(0–600%) 1000(100%) 290 ms [215]
7.25(600–1500%)
13.45(1500–4800%)
PAM/PDA/pGO 400% / / / / [213]
PVA/DMSO/rGO/GO(PDRG) ~600% 3100 2.21(0–600%) 4000(50%) 250 ms [82]
PAM/PAA/graphene /PEDOT:PSS 500% 150 0.77–100(0–160%) 1000(60%) 366 ms [219]
1–1.6(160–500%)
graphene/AA/MEA 500% / 0,62(0–20%) 500(50%) / [194]
0.98(20–100%)
1.83(100–300%)
3.4(300–500%)
graphene/PVA/PAA / / 39(50%) 5000(5%) 274 ms [220]
PVA-G-PDA-AgNPs 331% 1174 0.937(0–70%) / / [221]
0.13(>70%)
graphene/PAM/CA 500% / ~5(1–100%) 1000(100%) / [222]
1811.88 ± 112.44(200–500%)
GGOHX >500% >750 ~2.1(0–300%) 4000(30%) 150 [223]
~10.8(300–400%)
polyurethane (TPU),[107] graphene/polyvinylidene fluoride(PVDF)/ exceptionally high. However, these devices are not always good at
TPU,[141] GNPs/aramid nanofibers (ANFs)[142] or graphene/PDMS maintaining their performance and stability over time due to the poor
[143] were also synthesized via the wet-spinning process for making adhesion of these coating layers during stretching or bending processes.
strain sensors. Fibers made from the wet-spinning methods are primarily To solve this problem, encapsulation has been applied in many situa
composed of conductive and polymer matrix, which can be functional tions. For example, a spandex was firstly modified by a layered dipping-
ized as sensing elements and elastic components, respectively. drying procedure and subsequently encased in semi-permeable mem
Among the common spinning techniques used in the production of branes for strain measurement, which can be served as a protecting and
fibrous materials used in strain sensors, electrospinning is another most intermediate adhesive layer, respectively (Fig. 3d).[152] Several fiber-
commonly used one. In general, the fibers are electro-spun onto the based strain sensors have also been encapsulated in similar ways, such
polymer via incorporating one or more conductive fillers. However, this as TPU encapsulated PU composite fibers,[156] PDMS encapsulated
method often produces fibers with poor electrical properties. Alterna rubber (RY) and nylon covered rubber.[57] Additionally, surface mod
tively, conductive material can be applied to the fiber’s surface after ifications on natural fibers using conductive materials can form func
electrospinning elastic fibers. For example, using the electrospinning tionalized fibers to detect strains. Previous studies reported that rGO
SBS fibers, Taromsari et al. modified it with GNPs and Mxene (Fig. 3c), sheets coated onto hair for fabricating strain sensors are light and small,
[144] and reported that conductivity of the obtained sensors was and by harnessing the outstanding flexibility of hair, sensor-integrated
significantly increased during the surface modification process and gloves and 5 × 5 network arrays were made to detect bending of the
reached a value of 82.64 S/m after vacuum-assisted filtration and ul fingers and pressures, respectively.[157].
trasonic atomization processes. Some other methods using improved Conductive material-coated yarns have been investigated for their
electrospinning technology have produced similar strain-responsive potential use in developing linear strain sensors and integrating them
graphene-based fibers.[145,146] It is noteworthy that cracks have into strain-sensing devices. Coating the polymer with conductive ma
been designed on the nanofiber surface through pre-stretching to terials is one commonly used approach. For example, by using spray-
strongly immobilize the nanoparticles.[145] Besides, strain-detectable coating, GNPs-coated yarns (with a conductivity of ~ 5 s/m after sur
fibers have also been developed through dry spinning,[147,148] melt face modifications) were demonstrated for strain sensing after being
spinning,[149,150] and microfluidic spinning.[151]. attached to a commercial medical adhesive bandage (Fig. 3e).[158]
Owing to the merits of assembling flexibility and outstanding wear
3.2.2. Surface modifications ability, the modified yarns have been developed as a glove with inte
Surface modification of non-conductive fibers and yarns is an effi grated sensors for tracking finger movements. In a similar strategy, Li
cient and suitable method for generating fiber-based and strain-sensitive et al. measured human physiological signals by charging AgNW/GNPs-
wearable sensors. This can be realized by dip-coating, spraying, and modified oxygen plasma-pretreated polyurethane yarn (PUY) using a
surface deposition.[152-155] With this technique, strain sensors are layer-by-layer (LBL) assembly method for strain sensing (Fig. 3f).[159]
able to work in a wide range of strains, and the sensitivity is However, the stretchability of this strain sensor was limited to 125% as
8
Fig. 2. Graphene film-based strain sensors. Micro-structured conductive layers with a) fish-like, b) nanowall-like, and c) wrinkle-like. a) Reproduced with permission
[117]. Copyright 2016, American Chemical Society. b) Reproduced with permission [118]. Copyright 2020, Royal Society of Chemistry. c) Reproduced with
permission [104]. Copyright 2021, Royal Society of Chemistry. d) The fabrication of rGO/PDMS sensors via self-assembling. Reproduced with permission [119].
Copyright 2019, American Chemical Society. e) Durability of the LSG-based strain sensor with 10 000 cycles within 2% strain. Reproduced with permission [121].
Copyright 2018, American Chemical Society. f) Cyclic performance of CNFs/GNPs/PDMS strain sensor with 1000 cycles within 50% strain. Reproduced with
permission [122]. Copyright 2018, American Chemical Society. g) Durability testing the rGO and rGO/PDA/Ni strain sensors under 8% strain, respectively.
Reproduced with permission [123]. Copyright 2020, American Chemical Society. h) Preparation of the gradient wrinkle strain sensor via biaxial pre-stretching. i)
Response signal of the gradient wrinkle strain sensor in various environments. h,i) Reproduced with permission [104]. Copyright 2021, Royal Society of Chemistry.
the relatively hard polyvinyl alcohol(PVA) coating was used. This [164] Similarly, rGO-coated polyester wound spandex yarns were
concept has also been applied to graphene/Au[160,161] or graphene fabricated and demonstrated for the strain detection.[165] The perfor
[57,162,163] modified yarns. mance of these strain sensors with a helically covered structure can be
Intriguingly, the modified yarns covered elastic yarns and formed easily optimized through pre-stretching processes.
helix structures, which provide good strain sensing capabilities since the Various coating methods are commonly applied to enhance fibers
modified yarns are separated and in contact with one another. For with diverse capabilities, and they present numerous benefits such as
example, Fig. 3g shows a graphene-based composite fiber based on a ease of forming continuously coated layers, simplicity of fabrication,
double-covered yarn with a spring-like architecture, which is composed and scalability of the process. However, the adhesion between conduc
of a helically winding covered layer and the PU core. As the tensile strain tive layers and substrates is normally realized through hydrogen
is applied, gaps are created during the elongation of the fiber surface, bonding, which can negatively affect its adhesion and durability. A
reducing the contact area and increasing the sensitivity of the sensor. promising strategy is to add a protective layer around the conductive
9
Fig. 3. Graphene fiber-based strain sensors. a) Wet-spinning process for fabrication of hybrid fibers with core − shell. Reproduced with permission [139]. Copyright
2020, American Chemical Society. b) Fabrication of SBS/FLG composite fibers by wet-spinning and photograph of fibers containing 5 wt% FLG. Reproduced with
permission [140]. Copyright 2018, Elsevier. c) Electrospinning SBS fibers modified with graphene and MXene for strain sensing. Reproduced with permission [144].
Copyright 2022, Elsevier. d) Illustration of semi-permeable membranes encapsulated spandex. [152] e) The fabrication of GNPs-coated yarns via spray-coating.
Reproduced with permission [158]. Copyright 2019, American Scientific Publishers. f) Illustration of AgNW/GNPs/PUY strain sensor with LBL assembly. Repro
duced with permission [159]. Copyright 2022, Springer Nature. g) The production of a spring-like strain sensor. Reproduced with permission [164]. Copyright 2015,
Wiley-VCH.
layer, such as PVA and PDMS.[163,166] Nevertheless, this method exhibits a good stability in the cycling test.[167].
cannot address the fundamental problems such as poor adhesion, and it Despite these two promising approaches, the development of fiber-
also involves a lot of issues such as reduced flexibility and spinnability. based strain sensors still faces some obstacles. In the preparation of a
Thus, a solution that can create a strong covalent bonding between the spinnable composite formulation using an elastomeric host and a filler,
coating layer and elastic substrate through surface modifications was many technical challenges are existed. This requires aggregation-free
recently proposed, which not only strengthens the adhesion but also dispersion of high quality, low-particle size and high concentration of
10
graphene fillers. Furthermore, augmenting the interactions between 3.4. Hydrogel-based strain sensor
graphene and elastomer matrix is another barrier, as the deposited
conductive layer in the strain sensor is easily washed away from sub Hydrogels are hydrophilic crosslinked polymer networks with high
strates, causing poor performance in applications. New approaches are water contents.[191] A major advantage of using hydrogels is that they
urgently needed to achieve a high cyclic stability with mechanical are mechanically similar to bio-tissues.[192,193] However, hydrogel
properties similar to those of the original fibers. exhibits a significantly lower intrinsic electric conductivity than those
traditional conductive materials, making it ineffective as an electrical
3.3. Foam-based strain sensor stimulus and signal transmission medium. To enhance the electrical
conductivity, attempts to introduce graphene into nanocomposite
Despite having obtained significant achievements, the problem of hydrogels, as a reinforcement and conductive filler, have been increased
homogeneous dispersion of graphene sheets remains unsolved, which drastically in recent years. As illustrated in Fig. 5a, by combining syn
becomes a key barrier for obstacle to unleash the excellent potentials of ergistic hydrophilic and hydrophobic network structures which are
graphene.[175,176] To address this problem, a novel three-dimensional responding to organic solvents and aqueous solutions, the graphene-
(3D) network comprised of graphene foam with a high porosity and assisted hydrogel presents superior performance including adhesive
large surface area was proposed for a variety of applications including and anti-freezing behavior, and solvent-resistant and non-swelling
absorbents and energy storage.[177-180] However, due to the brittle properties.[194] Even though graphene-based hydrogel sensors have
ness in bending or stretching exhibited in most of the reported graphene made some notable progress, they face some major challenges. For
foams,[181] their widespread applications were restricted. Therefore, example, graphene nanosheets are susceptible to aggregation in the
the uses of various polymer reinforcements are crucial for graphene hydrogel, especially when using mechanical blending methods, result
foams to obtain excellent flexibility and tensile properties.[181,182] ing in a poor performance.[195-197] Moreover, the interactions be
There are currently several techniques available for construct 3D gra tween graphene sheets and hydrogel matrix are weak, restricting the
phene foams, such as CVD, template-assisted, and self-assembly pro transfer of stress effectively to polymers.
cesses. [95,183,184] Both the CVD and template-assisted methods Recent studies have shown that adding oxygen-containing groups
require porous templates such as nickel or Cu foams, which need to be onto graphene (e.g., GO)[198] was effective in promoting the dis
etched away in the subsequent processes to obtain pure graphene foams. persibility of graphene, thereby strengthening the polymer networks’
Using different templates, network and porous structures of graphene interactions. The use of GO nanosheets in the manufacture of tough
foams can be tuned. For instance, when Cu is applied for a template hydrogels[199-201] and shape memory hydrogels,[202-204] as an
skeleton, the generated graphene foams tend to collapse or fracture, efficient enforcement and physical crosslinker, has been extensively
simply because its building blocks (i.e., monolayer graphene) cannot explored in recent years. Unfortunately, the oxidization process of gra
withstand the liquid capillary forces generated by acetone evaporation. phene under a harsh chemical condition or at a high temperature
[185] Many studies have shown that Ni templates are promising for severely disrupts the conjugated structures, which negatively impacts
solving this issue.[186,187]. the conductivity of GO-based hydrogels. One effective method of
Carbon-containing gases are commonly used as a source for growing embedding GO in nanocomposite hydrogels is to introduce ions which
graphene on templates in CVD, where the gas concentration has sig are served as conductive elements, and the GO can be used as a rein
nificant effects on the amounts of graphene layers, the density and forcing agent to boost the mechanical performance.[80,203,205] For
specific surface area of graphene foam. The template-assisted method is example, polyacrylic acid (PAA) hydrogels containing GO, FeCl3, and
based on aqueous solutions. A method of CVD-growing graphene foam chitosan (CS) were prepared with a binary solvent of water and glycerol
and graphene foam-PDMS composites have been reported by Chen et al. to generate anti-freezing and self-healing properties (Fig. 5b).[80] In the
(Fig. 4a).[185] In brief, at an ambient pressure of 1000 ◦ C, CH4 was presence of –COOH and –OH groups, GO could not only be served as a
pyrolyzed, and three layers of graphene films were precipitated on the bridge connecting PAA and CS, but also be crosslinked with Fe3+ ions. As
surface of the nickel template, and the skeleton was etched away in a hot well as providing electrical conductivity to the hydrogels, FeCl3 en
HCl solution subsequently. All the graphene sheets in the graphene hances the strain sensitivity, while glycerol lowers the freezing point of
monoliths were directly contacted among each other, preserving the water, thereby conferring anti-freezing properties to the hydrogel.
interconnected 3D framework inherited from the nickel foam template. With good water solubility and considerable conductivity, rGO, as an
Similar graphene foams have been successfully produced by utilizing alternative to using GO, can be used to prepare conductive nano
different preparation sequences and/or different conditions in other composite hydrogels for sensors.[206-209] Many chemicals have been
groups.[95,184,186,188,189] For example, a flexible and self-healing applied to prepare rGO sheets, including hydroiodic acid (HI),[210]
strain sensor has been developed by incorporating functionalized poly polydopamine(PDA)[211,212] and hydrazine hydrate[208]. Its
urethane (FPU) elastomer into thiolated graphene foam (TGF) with sil biocompatibility, non-toxicity, and mild reduction conditions make PDA
ver nanowire (AgNW) coating (Fig. 4b).[189] After cut into two one of the most promising agents. Fig. 5c shows a highly stretchable and
separate pieces and sealed together, the healed sensor’s resistance was self-adhesive hydrogel compose of partially reduced GO (pGO) and
returned back to its original value and remained stable values during the polyacrylamide(PAM).[213] Besides improving the toughness of
contact-separation cycles, as shown in Fig. 4c-d. Self-assembly methods hydrogel, pGO also enhanced its conductivity. With its good biocom
for graphene foams typically start with GO and are then completed by patibility, it can be implanted into body in vivo without causing any
drying processes, including using oven [180] or freeze-drying.[183] For inflammation. The PAA–rGO nanocomposite hydrogel was also fabri
instance, Li et al.[190] prepared graphene foam with ultra-low density cated using PDA as a reducing agent by Jing et al., with pressure- and
(4.5 mg cm)-3), high porosity (99.8%) and medium GF (98.66 at 5% strain- sensitive features.[214] Furthermore, poly(3,4-
strain) using a self-assembly process under mild conditions (Fig. 4e). ethylenedioxythiophene)(PEDOT) composite nanosheets with
In general, strain sensors based on graphene foam have demon sandwich-like structures, which were obtained by assembling PEDOT
strated limited sensitivity and a restricted strain range. This is because onto polydopamine-reduced and sulfonated graphene oxide (PSGO),
although foams are conductive, their conductor paths are hard to change have been combined with PAM network. This can achieve wearable and
when deformed. Besides, achieving precise control over the structures of implantable bioelectronics that showed a high conductivity (108 S m− 1)
graphene foam, including their pore sizes and porosity, is a challenging and a wide working range (2000%), as depicted in Fig. 5d.[211]
task. Additionally, the strain sensor’s breathability is compromised Additionally, it should be addressed that the above two approaches
when it is filtered with elastic polymers, as the lack of pores within the can be combined into one hydrogel at the same time, creating a syner
material causes this effect. gistic effect and resulting in a denser network and higher conductivity in
11
Fig. 4. Graphene foam-based strain sensors. a) Synthesis of a graphene foam, integration with PDMS and photograph of a bent graphene/PDMS composite.
Reproduced with permission [185]. Copyright 2011, Springer Nature. b) The fabrication, c) the self-healing ability, and d) the contact − separation cycle process of
the AgNWs@TGF/FPU strain sensor. b,c,d) Reproduced with permission [189]. Copyright 2020, American Chemical Society. e) Illustration of the graphene foam
infiltrated with PDMS via self-assembly. Reproduced with permission [190]. Copyright 2016, American Chemical Society.
12
Fig. 5. GO hydrogel-based strain sensors. a) A graphene-assisted hydrogel with solvent-resistant and non-swelling properties. Reproduced with permission [194].
Copyright 2020, American Chemical Society. b) GO-reinfored PAA hydrogel with FeCl3 and CS under binary solvent. Reproduced with permission [80]. Copyright
2019, Royal Society of Chemistry. c) pGO-PAM conductive hydrogel with adhesion and self-heal ability. Reproduced with permission [213]. Copyright 2017, Wiley-
VCH. d) Design and assembly of sandwich-like PSGO–PEDOT nanosheet based-hydrogel. Reproduced with permission [211]. Copyright 2020, Wiley-VCH. e)
Fabrication process of double-network nanocomposite hydrogels with GO fillers and Ca2+ crosslinker. Reproduced with permission [210]. Copyright 2019, Royal
Society of Chemistry.
the nanocomposite hydrogel.[82,213,215] As shown in Fig. 5e, a temperature, hydrogels are not immune to water loss, which leads to the
double-network nanocomposite hydrogel with GO as conductive fillers degradation of the prepared sensors and hinders their development in
are utilized to fabricate wearable biosensors by treating with HI vapor various fields. Finally, due to the lack of adhesion, the hydrogel can
for enhancing conductivity.[210] A noteworthy addition to the network easily be detached from the body, especially with continuous secretion
is the introduction of Ca2+, which can be applied as a dynamic and of grease and sweat by the body, which generates a huge noise in re
reversible crosslink between adjacent GOs and a link between PAAs and sponses or may lead to complete failure. Therefore, future research
GOs. should not only be limited to improving the sensitivity of hydrogels, but
Even though the good performance of GO/rGO based nanocomposite also be focused on manufacturing hydrogels with excellent mechanical
hydrogels in terms of stretchability has been achieved, there are still and electronic properties, good adhesion ability and stability in high and
some critical issues remained. Firstly, if comparing with sensors using low temperature environments.
the conventional elastomers, the sensitivity of hybrid hydrogels is quite In summary, graphene and graphene related materials can signifi
low, generally <10. Secondly, the hydrogels lack environmental sta cantly enhance the overall performance of strain sensors, especially the
bility, and their water contents could be evaporated easily at high mechanical and electrical properties. In terms of mechanical properties,
temperatures and frozen easily at subzero temperatures. Even at room the exceptional strength of graphene can be utilized to improve the
13
deformation adaptability of the tensile strain sensors. For instance, the The researchers showed that resistance changes are correlated with the
graphene foam-based strain sensors usually show superior mechanical blink frequency, which is increased rapidly when the eye is overused
robustness due to the π–π interfacial interactions between graphene from 30 min− 1 to 87 min− 1(Fig. 6c). As a result of excellent sensing in a
nanosheets.[216] Nevertheless, for the fiber-based strain sensors, gra variety of environments, these sensors can monitor or prevent many
phene nanosheets are easily restacked and aggregated during the spin types of eye diseases, including dry eyes caused by chronic computer
ning process due to the van der Waals force among nanosheets. For fatigue. Attaching an rGO composite hydrogel sensor on the eye can
hydrogel-based sensors, the accumulation of graphene in the precursor detect subtle facial expressions like frowning and smiling (Fig. 6d).[218]
solution is often quite severe, which significantly affects the mechanical Moreover, wearable strain sensors are competent to measure the
properties of the prepared hydrogels. Therefore, GO with its impressive epidermal vibrations of the throat caused by swallowing, drinking
dispersibility is often used as a reinforcing component to enhance the water, coughing and speaking.[81,118,203,220,226,236,237] As
toughness and ductility of hydrogel sensors. demonstrated in Fig. 6e, strain sensors can assist with speech rehabili
For electrical properties, graphene is well-suited for constructing tation based on the different and repeatable signals generated by
ultra-high sensitivity strain sensors. In general, the content of graphene speaking a few English words.[238].
nanosheets can significantly affect the electrical properties of sensors,
especially for those film and fiber-based sensors. Graphene derivatives, 4.2. Applications for health indicators
such as GO, have poor electrical conductivity, therefore, the sensitivity
of GO-based strain sensors is often unsatisfactory. To improve conduc It is crucial and indispensable for the management of public and
tivity, GO can be easily changed into rGO using thermal or chemical personal health in the contexts of epidemiology and disease control. The
treatments. For hydrogel-based sensors, their excellent electrical and high limit of detection (LoD) for graphene-based flexible strain sensors
mechanical properties can be obtained simultaneously by controlling enables them to detect vital signals, such as heartbeat, pulse, and
the degree of reduction of GOs. respiration, making them as ideal health indicators in an accurate and
unobtrusive manner.[74,116,239] In Fig. 6f, an example of sensor de
4. Applications signs for detecting the pulses of the wrist and finger is illustrated by
placing sensors (constructed from laser induced graphene) on the wrist.
Graphene-based stretchable sensors have demonstrated significant [114] Repeatable and regular shapes reveal the frequency of the wrist
potentials in numerous fields, most notably for the applications of pulses, e.g., about 70 pulses min− 1, corresponding to a healthy heart
human motion sensing, health indicators, human–machine interfaces, beat. An individual pulse consists of three characteristics, namely the
and electronic skins. The applications of graphene-based flexible strain percussion wave (P-wave), tidal wave (T-wave), and diastolic wave (D-
sensors are discussed in this section. wave), which doctors can use for diagnosis of various diseases.
By means of flexible strain sensors based on graphene, some essential
4.1. Applications for human motion sensing prognostic information regarding heart diseases and blood pressures can
be observed, for example, jugular venous pulse (JVP). An application of
A surge in demand for real-time monitoring of human activities has strain sensors with black phosphorous-supported with CO2 laser-
arisen in recent years. Unlike the traditional metallic or semiconducting engraving graphene is shown in Fig. 6g.[238] The JVP waveform pro
strain sensors with a narrow stretchability, graphene-based flexible vides key information about the breathing rate (e.g., 12 breaths per
sensors are available for working in a wider range of strains. minute) and cardiac conditions (e.g., 62 beats per minute), suggesting
[52,224,225] By applying graphene-based stretchable sensors on that this technique has potential applications in surveilling apnea among
different body parts, the deformation movements of the body can be grown-ups and screening for sudden death syndrome in neonates. Gra
tracked continuously. The vigorous movements which can be monitored phene strain sensors can also be assembled on a face mask to measure
include bending of limbs or stretching movements, whereas those deli human breathing, as shown in Fig. 6h, in both a relaxed state (19
cate motions include emotional expression and swallowing. breaths/minute) and during exercise (80 breaths/minute).[120].
For detection of large-amplitude signals, such as those generated by
human fingers or knees bending, ideally, the wearable strain sensors 4.3. Applications for E-Skin
should offer a wide sensing range. For example, as shown in Fig. 6a, a
multifunctional flexible sensor was mounted on the nape for continuous Skin, as a tissue in direct contact with the external environment, can
monitoring of head movement.[226] With real-time monitoring fre perceive a variety of external stimuli at the same time. Its fascinating
quency of the motion of children’s heads, it is possible to assess their properties, such as self-healing ability, have been already extensively
level of attention by detecting the resistance signals of the sensor explored. Regarding artificial intelligent skin, graphene-based flexible
responded to the directions and amplitudes of the head’s rotation. Be strain sensors, with a combination of the superiorities of substrate
sides, taking advantage of its notable electrical and stretchability, these (stretchability and biocompatibility) and graphene (conductivity), are
strain sensors are capable of measuring changes in electrical signals as a ideal candidates. To fully realize the functions of human skin, several
result of bending fingers, wrists, arms and various complex movements. graphene-based strain sensors with multi-sensing abilities (e.g., strain
[173,194,227-231] Typically, detection of hand gestures by the changes and pressure,[129,130,153,240] temperature and strain
in the electrical signal of the sensor generated by finger flexion in a glove [82,128,235,238]) have been designed. Using conductive hydrogels and
sheds a light on the field of sign language recognition. thermochromic elastomer as active sensing components, a dual-sensory
[102,116,212,232] Fig. 6b exhibits a dual-network conductive hydrogel sensor which couples with different sensing mechanisms has been re
encapsulated in CNTs/PDMS films for measurement.[219] Finger ported for detecting both body movement and temperature changes
bending increases the relative resistance, which can be returned to its through a dual-core coaxial wet-spinning process (Fig. 7a).[139] Simi
original state in accordance with the corresponding motion inputs. In larly, Fig. 7b shows a degradable and recyclable paper-based strain
addition to the above-mentioned examples, several body movements, sensor which is consisted of carbon black (CB) and rGO as a hierarchical
such as waist-related motions and squatting, were also captured in real- sensitive layer for monitoring various stimuli.[240] The paper-based
time by means of flexible strain devices.[151,233,234]. multimodal sensor was fabricated via a spraying technique, which can
The sensitivity and accuracy of strain monitoring are essential when achieve a good conductivity. However, due to the high mobility of the
it comes to weak strain signals generated by small-amplitude. Previously conductive network, the sensor is susceptible to changes of its con
a dual-mode sensor constructed from graphene foam has been intro ducting routes when subjected to various external stimuli (e.g.,
duced, which was applied to the eyelid to detect blink frequency.[235] humidity-induced swelling of the sensing layer and pressure-induced
14
Fig. 6. Applications for human motion sensing and health indicators detection. a) The surveillance of head rotation by mounting a strain snesor on nape. Reproduced
with permission [226]. Copyright 2018, Royal Society of Chemistry. b) Dection of finger bending throug the hydrogel-based sensor. Reproduced with permission
[219]. Copyright 2022, American Chemical Society. c) Recognition of a blink rate by attaching a strain sensor on the eyelid. Reproduced with permission [235].
Copyright 2022, Elsevier. d) Detecting changes in volunteer expressions. Reproduced with permission [218]. Copyright 2021, Royal Society of Chemistry. e)
Phonation when the wearer spoke “Sensor” and “Congratulations”. Reproduced with permission [238]. Copyright 2021, Wiley-VCH. f) A strain sensor for detecting
wrist pulse. Reproduced with permission [114]. Copyright 2019, Wiley-VCH. g) The dection of JVP with respiration and holding respiration. Reproduced with
permission [238]. Copyright 2021, Wiley-VCH. h) A sensor fixed on mask for respiration detection. Reproduced with permission [120]. Copyright 2017, Royal
Society of Chemistry.
15
Fig. 7. Applications for E-skin. a) Dual-sensory sensor for detecting strain and temperature. Reproduced with permission [139]. Copyright 2020, American Chemical
Society. b) CB/RGO/paper sensor for detecting multiple stimuli. Reproduced with permission [240]. Copyright 2019, American Chemical Society.
condensation of the conductive layer), resulting in changes in current or strain sensor based on graphene/PDMS and introduced strain in
resistance. Graphene-based devices still do not have simple but effective teractions between human and robotic arms (Fig. 8b). The wearable
methods to detect multiple signals simultaneously. Upon receiving strain sensor can convert resistance changes into signals, which controls
external signals, the human skin is capable of working collaboratively or the robot to make different movements.
independently and identifying different signals. Hence, the development Combining wearable electronics and wireless transmission technol
of electronic skins needs to be further advanced to enable real-time ogy with the benefits of low power consumption can provide a simple
detection and discrimination of multiple signals, thus fully emulating and effective bridge between human and machines and facilitate the
the functioning of human skin. wearable HMI process. Fig. 8c presents a schematic graph of wireless
monitoring for human activities using a Bluetooth connection.[232] The
4.4. Applications for Human-machine interface glove was equipped with five strain sensors, and the responses of each
finger could be distinguished from one another, making it possible to
The wearable human–machine interface (HMI) facilitates informa identify gestures. Volunteers wearing gloves can synchronize their
tion transfer between humans and machines through the collection of hands’ movements to the cell phone. Zhai et al.[171] constructed a real-
physical signals from consumers and directing the machine to execute a time motion monitoring system based on flexible strain sensors
specific task. In contrast to the conventional terminal control mecha (BWWAJ) using twisted graphene fiber. Fig. 8d-e show the applications
nisms (such as keyboards and touchpads), graphene-based flexible of the BWWAJ strain sensor and Bluetooth transmission module in
sensors enable human–machine emotional interactions that are more human motion detection.[171] The movement signals of the elbow and
innovative but complex. In terms of interactive technology, gestures knee joints in different strokes are displayed on the mobile interface, and
have the potential to offer a more intuitive, natural, and creative means the anomalistic patterns of the signals in terms of amplitude and fre
of communicating with machines.[83,215,241,242] For example, Zhou quency indicate that the swimmer is in a potentially dangerous
et al. [215] recently proposed a self-adhesive and superior stretchable situation.
hydrogel (SPGCP) with a hierarchical configuration. They integrated the
SPGCP glove, a microcontroller unit (MCU) that records and processes 5. Challenges and future directions
the signal, and a robot hand that communicated with MCU via RF
wireless (Fig. 8a). The robot’s hand was shown to be synchronized and Even though there have been various advanced materials and
manipulated by human gestures and demonstrated the ability to perform structures which have been developed to enhance the performance of
more complicated movements. Similarly, Luo et al.[83] developed a graphene-based stretchable strain sensors, various problems are still
16
Fig. 8. Application for HMI. a) The SPGCP hydrogel integrated glove for controlling robotic arm. Reproduced with permission [215]. Copyright 2022, Elsevier. b)
The graphene/PDMS sensor for controlling robot dancing. Reproduced with permission [83]. Copyright 2020, Wiley-VCH. c) A glove integrated with strain sensors
for gesture recognition. Reproduced with permission[232]. Copyright 2022, Royal Society of Chemistry. d) Illustration an underwater wireless monitoring for human
activities. e) Electrical signals of various swimming strokes. d,e) Reproduced with permission [171]. Copyright 2022, Elsevier.
17
remained and urgently needed to solve before their practical In addition, the involuntary physical presence of water vapor in the
applications. human body by the respiratory pathway will generate sweat on the skin
surface. This respiratory breathing pathway becomes more active when
5.1. Improved properties the person is doing exercise. The efficiency of vapor transport is often
affected by the interface between the elastic polymer and the skin. To
The grand challenge is to improve the overall performance of the improve the breathability of the sensors, designing conductive
sensor instead of over-utilizing each single property. In current study, materials-based textiles or 3D sponges are effective strategies which
attention is focused on performance metrics (e.g., stretchability and allow the sweat to be evaporated through the porous structure.
sensitivity) and huge progress has been made so far. Since the signals Currently, several approaches are available to obtain ultra-thin breath
from sensors are easily amplified via specific electric apparatus, a wider able devices, including electrostatic spinning, etching, and thin film
sensing range becomes more critical compared with the improvement of preparation.
its sensitivity. Therefore, more vigorous studies should be done to Besides wearing comfortability, good biocompatibility is essential
develop strain sensors which show both outstanding GF and a large for the practical application of on-dermal and implantable strain sen
stretching range. To tackle this issue, several techniques are currently sors. This can effectively avoid the hazards led by immune rejection and
applied. For instance, for the crack-propagation based strain sensors, is thus valuable for long-term detection. When using flexible sensors in
bridging materials (e.g., AgNWs and CNTs) can be incorporated into the wearable systems for physiological signal detection, much more atten
matrix to improve effective structural connection. Whereas for the strain tion should be paid to biocompatibility and adhesion.
sensors based on disconnection mechanisms, solid lubricant (e.g., C60)
can be added to reduce the applied stress. 5.3. Robust anti-jamming
Another critical issue in strain sensors is the linear correlation be
tween strain deformation and electrical signal outputs. For non-linear The immunity characteristics and other ancillary features of strain
sensors, more sophisticated transformation functions are required to sensors are equally important for wearable applications. As we have
perform proper interrogation. This results in the sensor with inhomo addressed before, for most reported strain sensors, significantly different
geneous resistance over the entire dynamic range, thereby often limiting responses were obtained when faced with various types of deformations.
its application. Further research is needed to explore and validate the It is a great challenge to precisely detect motions in wearable conditions,
linearity mechanism over the entire large sensing range. For example, especially under complex moving conditions or within noisy back
the microstructure inhomogeneity of the sensor material needs to be grounds. Hence, anti-jamming properties-strain sensors to the mechan
modified in order to construct uniform cracking patterns in film-based ical stimuli are of great significance to precisely detect motions in real-
strain sensors.[84]. time. Motions perceived in noisy backgrounds can be addressed by cir
More importantly, it is vital to develop multiple electromechanical cuit optimization (e.g., filters and amplifiers) and data processing. To
properties including hysteresis, stability, and durability, which show a extract the real signals, an initial threshold can be set, and then the
good detection accuracy and lifetime, but this issue has not been paid output signals below this initial threshold can be filtered out using a
much attention. Although signal processing and enormous character threshold evaluation algorithm. Meanwhile, multiple deformation
ization of the sensor’s responses can be used to minimize this problem, it modes from input stimulus can be detected and further decoupled with
is often troublesome for achieving these characteristics, and more the help of artificial neural networks.
studies are needed for optimization of stability and other performance. Wearable interfaces often experience dramatic changes of local
For improving the stability of the sensors, a brick-and-mortar structure temperature, humidity, pH values, and possible bacterial infections, thus
can be designed to reduce the unstable contacts between adjacent significantly deteriorating the sensor’s reliability. It is also commonly
nanomaterials through ionic bonds and π − π bonds. known that graphene is very sensible to the stimulation from wearable
Furthermore, both standardization of assessing responses and re microclimate. Therefore, exploring strain sensors that maintain good
covery times are of great significance. The comparison between response anti-jamming performance to the wearable micro-environments in
and recovery time can be conducted when the imposed magnitude and absence of affecting their intrinsic properties is highly desirable. To
the strain rate are standardized or fixed. Likewise, the sensitivity values achieve waterproof performance of film-based sensors, a super
are difficult to be compared since they are strongly dependent on the hydrophobic coating can be constructed on the surface (which could
strain ranges for which they are calculated. Whereas in some situations, have a large roughness and a low surface energy), thereby reducing the
scientists often used output signals beyond resistance (e.g., current), solid–liquid contact area.
therefore, when comparing the sensitivity values of different sensors, In view of the availability of strain sensors for the e-skin, they should
caution should be taken into consideration for these issues. be given various auxiliary functions such as multi-signal monitoring, air
permeability and self-sealing properties. For the preparation of multi
5.2. Enhanced wearability functional sensors, different sensing mechanisms can be integrated, such
as simultaneous detection of optical properties (e.g., light intensity) and
As we have addressed, wearability is an important assessment index electrical properties (e.g., resistance). The combination of liquids,
of wearable sensors. This involves three main aspects of adhesive, nanomaterials, and optical or optoelectronic materials facilitates the
comfortable, and biocompatible issues. The precondition in deciding its construction of such high-performance sensors for detecting various
reliability is focused on the conformal attachment of strain sensors on stimuli.
human bodies, but it is often critically underestimated the actual strain
and gives rise to severe motion artifacts. Many sensors still rely on non- 5.4. Advanced fabrication
stretchable tape or band-aids for attachment to the body to the body.
Adhesion is undesirable under different strain ranges and multi- The development of advanced fabrication approaches for graphene-
dimensional deformations. This causes inconvenience in the move based strain sensors is still in its early stages, and future progress in this
ment of body parts and unacceptable feeling of rejection in long-term direction is essential. Firstly, it is crucial to achieve highly efficient
usage. Strategies to effectively enhance the self-adhesion of the sen manufacturing of flexible sensors. Many conventional fabrication
sors (mostly inspired by the biological systems) include chemical ad methods have issues such as high processing costs and complicated
hesives (e.g., polydopamine), gecko-inspired microfibers, microneedle manufacturing processes. Therefore, there is an urgent need to investi
arrays with swellable tips, low modulus and miniaturized suction cups gate scalable, customizable, and environmentally friendly fabrication
and ultrathin packaging.[243]. processes for a large-scale production, such as using additive
18
manufacturing and printing technologies. They offer the possibilities to through the use of textile manufacturing technologies including
fabricate highly complex 3D structures, which can expand the applica weaving and knitting. To achieve uniform dispersion of graphene sheets,
tion areas of sensors. 3D graphene foam-based sensors with large surface area and high
Besides, it is essential to manufacture sensors with a high repeat porosity have been developed. Besides, based on hydrogels with supe
ability. For example, when these sensors are used as arrays, the varia rior softness and biocompatibility, flexible and stretchable graphene
tions among different sensors are significant, so that each sensor needs hydrogel-based strain sensors have been explored.
to be calibrated individually. This operation requires more complex For the production of graphene-based flexible/stretchable elec
circuitry to accomplish. As the number of sensors in an array is tronics, traditional processing methods based on solutions (e.g., spray
increased, the tolerance for inter-sensor variability is decreased signifi coating, dip coating, spinning, and layer-by-layer assembly) have been
cantly, thus making the sensing operation rather difficult. In the com widely developed. For instance, several novel printing techniques,
posite strain sensors, inter-sensor variability typically arises from the including screen printing, aerosol-jet printing, and laser pattering, have
aggregation and inhomogeneous dispersion of conductive materials in been applied as well as for synthesis of flexible/stretchable electronics.
the elastomeric matrix. This variability will be increased when the size Additionally, structural engineering was applied to optimize the per
of sensors becomes much smaller. To ensure the reproducibility of the formance of graphene-based flexible electronics, such as designs of
fabrication processes, a coupled printing technique can be adopted to scale-like, nanowall-like, wave-like, and wrinkle-like, which are essen
enable the large-scale production and affordability of graphene-based tial for the graphene-based flexible electronics used in practical
strain sensors. applications.
The graphene-based strain sensors has found various applications,
5.5. Intelligent integration including human motion sensing, health indicators, electronic skins, and
human machine interface. For example, such sensors can be attached to
External power sources and metal interconnections with other elec different parts of the human body for monitoring human health and
tronic devices are needed for many strain sensors used in practice. Self- activities, such as monitoring indicators including pulse, respiration,
powered and wireless networks offer more significant advantages in and vocalization. For future practical applications, advanced technolo
practical applications than wiring systems. It is noteworthy that high- gies, such as artificial intelligence (AI) processing, should be investi
performance and self-powered strain sensors are critically needed to gated within the interdisciplinary fields (e.g., virtual reality and sign
monitor long-term activity. For the power supplies of sensors, energy language recognition) for commercialization and practical application
harvesting from the environment and the human body (e.g., triboelectric of flexible electronic devices.
generators and thermoelectric generators) can significantly enhance Although noticeable progress has been achieved in the fabrication
power-compatibility and self-sustainability of strain sensors while methods, performance optimization, and application expansion of
minimizing their weight and space. Moreover, more functionalities graphene-based strain sensors, further exploration is still needed.
should be integrated into the platform of graphene-based strain sensors, Firstly, studies on micro/nanostructure designs and sensing mechanisms
which are intended to build smart and interactive wearable systems. A should be carried out to simultaneously achieve multiple properties,
compact, functional, and reliable packaging process presents a major such as high stretchability and sensitivity. Besides, further development
adversity owing to the technical complexity of assembly, which includes of bio-inspired architectures requires extensive research on material and
a variety of functions such as displays, camouflage capabilities or data structural properties to enhance properties such as adhesion and con
storage/processing, as well as performance-dependent functions such as formability of devices. Moreover, the immunity and other ancillary
structural coloration and electroluminescence. In view of this, thin and characteristics of the strain sensor should also be considered. Achieving
flexible printed circuit boards with good bendability are suitable for a high repeatability is also a pivotal consideration in the effective
these applications, but with a rather limited market. Combining flexible manufacture of strain sensors, which has yet to be extensively studied.
wearable sensors with passive wireless technologies such as near-field Last but not least, it is still a formidable hardship to integrate sensors
communication with wireless, battery-free and multimodal monitoring into various devices or miniaturization of smart wearable devices. We
is currently another hot research topic, where the sensors can be easily strongly believe that the development of advanced graphene-based
deployed in arrays to achieve the low cost. wearable and flexible strain sensors for the next-generation healthcare
systems can be greatly facilitated by technologies for the design and
6. Conclusions manufacture of flexible electronic devices.
This paper summarizes the recent breakthroughs in the reasonable Author contributions
design methodologies, control parameters, synthesis and adhibition of
varieties of graphene and related materials toward wearable electronics The manuscript was written through contributions of all authors. All
with high-performance flexibility. Because of their extraordinary prop authors have given approval to the final version of the manuscript.
erties (e.g., ultra-translucency, good electrical conductivity, superior
mechanical flexibility, installation to be designed into different pliable Declaration of Competing Interest
macroscopic morphologies, and easily to being functionalized), gra
phene and related materials such as graphene, GO and rGO enable wide- The authors declare that they have no known competing financial
range applications in high-sensitivity strain sensors, which are prom interests or personal relationships that could have appeared to influence
ising for motion sensing, health indicator, E-skin, and HMI. the work reported in this paper.
Considering the great demands of diverse sensors and flexible elec
tronic units else, we have discussed the controlled micro/nanostructures Data availability
and macroscopic-morphology designs of graphene and related mate
rials. Functional groups and doping strategies have been used, resulting No data was used for the research described in the article.
in the successful demonstrations of diverse flexible electronics.
Combining material and structural designs, graphene film-based strain Acknowledgements
sensors offer optimized properties such as remarkable sensitivity and
repeatability. For the wear comfortability and outstanding lifetime of This work was supported by the Excellent Youth Fund of Hunan
fibers, sensors based on graphene fiber are the optimal selection for Province (2021JJ20018), the NSFC (No. 52075162), the Program of
textile strain sensors as they can be expediently switched into fabrics New and High-tech Industry of Hunan Province (2020GK2015,
19
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Chemical Engineering Journal 464 (2023) 142576

Contents lists available at ScienceDirect

Chemical Engineering Journal

Advances in graphene-based flexible and wearable strain sensors

1. Introduction developing such wearable strain sensors include incorporating con

PEI-rGO/PDMS Self assembly / 1744(5%) 6000(2%) / [119]

FLG/SBS Wet-spinning 700% 160 (0–50%) / / [140]

PAM/SF/GO/PEDOT:PSS (PSGP) 600% / 0.8(0–50%) 2000(50%) 170 ms [81]

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Graphene Wearables

Uploaded by

Copyright:

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Graphene Wearables

Uploaded by

Document Information

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Original Title

Copyright

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Graphene Wearables

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Chemical Engineering Journal 464 (2023) 142576

Contents lists available at ScienceDirect

Chemical Engineering Journal

Advances in graphene-based flexible and wearable strain sensors

1. Introduction developing such wearable strain sensors include incorporating con­

PEI-rGO/PDMS Self assembly / 1744(5%) 6000(2%) / [119]

FLG/SBS Wet-spinning 700% 160 (0–50%) / / [140]

PAM/SF/GO/PEDOT:PSS (PSGP) 600% / 0.8(0–50%) 2000(50%) 170 ms [81]

You might also like

1. Introduction developing such wearable strain sensors include incorporating con