REVIEW

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Advances in Functionalized Applications of Graphene-Based

Wearable Sensors in Healthcare
Mahmuda Akter,* Habibur Rahman Anik, Shariful Islam Tushar, Imana Shahrin Tania,
Md. Kamrul Hassan Chowdhury, Shah Md. Maruf Hasan, and Bebe Fatema Bristy

30 billion back in 2022, at a com-

Graphene has earned significant attention in the present world due to its light pound annual growth rate of 19.1%
weight and extremely good conductive properties, which are used in different for medical science and healthcare.[1]
functional materials and smart devices. With skyrocketing demand, wearable These wearables include different types,
sensors are evolving with many essential functionalities and flexibility in use. such as smart watches, glasses, jewelry,
bandages, electronic textiles, wrist/chest
Moreover, wearable sensors can show some marvelous activities easily when bands, smart clothing, rings, a real-
they are incorporated with different nanomaterials and two-dimensional (2D) time glucose regulator, smart tattoos,
materials. Therefore, after the immense effort and diligence of scientists over face masks, and more.[2] In general,
the years, wearable sensors can successfully exhibit numerous potential wearable devices consist of different
applications, such as motion detection, artificial intelligence, prosthetic skin, blocks, including a substrate and elec-
trode, a power unit, a sensing unit,
intelligent robotics, and human-machine interface and interaction. With the
and a decision-making unit.[3] Wearable
rapid development of flexible, perceptible electrical devices, graphene-based sensors play a crucial role in wearable
wearable sensors play an eminent role in healthcare. In this work, a technologies by facilitating the detection
comprehensive overview of recent research on wearable sensors and of biometrics, collecting biological data
integrated systems for various sections of healthcare is demonstrated. Along from the wearer, and then adapting to
with discussing the basic properties of graphene and the fabrication methods the body’s requirements. The first wear-
able sensor in the healthcare sector was
for graphene-based wearable sensors, this work can help the scientists invented several decades ago, in 1960,
address them and set a projection for future studies. Wearable named the Holter monitor, which is still
graphene-based sensors have great potential to make healthcare facilities very useful in monitoring heart activity.[4]
more accessible and enhance the quality of sensing activities, which has Certainly, wearable sensors are the an-
enormous implications for the future of healthcare. alytical tools that integrate with wear-
ables by combining and collecting the
responses of point-of-care systems au-
tomatically with built-in units.[5] Such
1. Introduction sensors can efficiently detect a very small change in physiolog-
ical response and excellently monitor the biometrics of the hu-
Wearable technology has been a booming industry, with an an- man body in a regular manner.[6] Wearable sensors have gained
ticipated global market worth USD 165 billion by 2030, up from significant popularity in the fields of disease detection and mon-
itoring, as well as in many healthcare and fitness applications. At
M. Akter, H. R. Anik, S. I. Tushar, M. K. H. Chowdhury, S. M. M. Hasan, present, wearable sensors are not only confined to human body
B. F. Bristy
applications but also expand their reach to the healthcare of live-
Department of Apparel Engineering
Bangladesh University of Textiles stock and pets.[7] Besides, wearables have made healthcare facil-
Dhaka 1208, Bangladesh ities more affordable, which increases their popularity and ac-
E-mail: [email protected] ceptability among the masses.[8] Also, wearable sensors are more
I. S. Tania user-friendly and easily accessible than the conventional clinical
Department of Wet Process Engineering diagnosis system.[9]
Bangladesh University of Textiles
Tejgaon, Dhaka 1208, Bangladesh In this current era, various types of wearable sensors are be-
ing intensively utilized and developed in the medical field for the
The ORCID identification number(s) for the author(s) of this article
can be found under https://doi.org/10.1002/adsr.202300120
well-being of humans and animals. Textile-based, paper-based,
hydrogel-based, etc., are the common sorts of wearable sensors
© 2023 The Authors. Advanced Sensor Research published by
Wiley-VCH GmbH.. This is an open access article under the terms of the in the health sector.[10] Besides, nanoscale materials like metal-
Creative Commons Attribution License, which permits use, distribution lic nanowires,[11] carbon-black elements,[12] nanoparticles,[13] car-
and reproduction in any medium, provided the original work is properly bon nanotubes,[14] nanorods,[14c,15] and also graphene,[16] can
cited. be utilized in developing stretchable and flexible wearable sen-
DOI: 10.1002/adsr.202300120 sors by coupling with elastomers for adequate sensitivity. Since

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Figure 1. An outline of graphene-based sensors for diverse applications in healthcare.

the very first invention of single-layer graphite through me- vironmental signals, as well as effective devices for the nervous
chanical exfoliation back in 2004, graphene has garnered a sig- system, cardiovascular sections, digestive systems, and locomo-
nificant amount of attention.[17] Graphene, a two-dimensional tor areas. However, persistent endeavors are currently under-
material,[18] has many desirable properties, such as high elec- way to adapt and augment the functioning of materials based
tron mobility through the material (350 000 cm2 (Vs)−1 ),[19] on graphene for specific sensing applications through differ-
thermal conductivity (5300 Wm−1 K−1 ),[20] Young’s modulus (1 ent innovative approaches.[26] For example, Qing et al.[28] inte-
TPa),[21] superior specific surface area (2600 m2 g−1 ), and reduced grated silk nanofiber to increase the conductivity and biocom-
thickness (0.34 nm).[22] Among all these amazing attributes, patibility of the rGO scaffold for tissue engineering. Graphene-
graphene’s thermal conductivity is one of the most effective in based wearable sensors are utilized for different purposes in
comparison to other common materials (i.e., even higher than the healthcare sector, such as health monitoring (i.e., pres-
metals and carbon nanotubes).[23] Thus, graphene and its deriva- sure sensing[29] ), human motion monitoring,[30] electrophysi-
tives can play a significant role in developing wearable sensors.[24] ological signal monitoring,[31] electronic skin and multifunc-
They can easily make the bridge between the sensors and the tional sensing,[32] temperature sensing,[33] and more. Noticeably,
device itself. These materials could be integrated into a multi- graphene-based wearable sensors can also make a revolutionary
layer stack to create heterostructure-based, multifunctional de- contribution to pandemics like COVID-19 by sensing and mon-
vices with exceptional characteristics and function control. Re- itoring viral infections.[34] In the future, the potential of wear-
searchers and individuals are taking an active role in using the able electronics with graphene sensors for telemedicine is signif-
unique features of graphene to produce sensors that can effi- icant, owing to the utilization of advanced technologies involving
ciently and rapidly detect and convert minute variations in an graphene-based materials.
open system. Additionally, efforts are being made to optimize its In this article, the development of graphene-based wearables
utilization in the healthcare industry. and recent trends in human health monitoring have been
Wearable sensors in the healthcare sector essentially must comprehensively reviewed. This review illustrates how fast
maintain optimal mechanical flexibility as well as outstanding the latest advancements have happened in graphene-based
sensing ability for comfort and proper integrity with the hu- wearable devices, with a particular emphasis on fabrication,
man body.[25] In this case, the graphene-based materials, in- features, and significant wearable applications. Different types
cluding graphene, graphene oxide (GO), and reduced graphene of fabrication techniques for graphene-based wearable sensors
oxide (rGO), are performing excellently as healthcare wearable in healthcare applications are discussed. The wide applications
sensors due to their outstanding biophysical and biochemical of wearable graphene-based sensors in the medical sector
sensing abilities along with ultrahigh flexibility.[26] Graphene- are thoroughly described, as is the sensing mechanism for
based materials are an appropriate carrier that can be trans- monitoring health issues. Recent developments in graphene
formed into a chemical sensor to detect fluids and gases be- devices have been discussed, along with the challenges they
cause of their extremely high specific surface area. Highly flex- present and possible approaches to resolving those challenges
ible graphene-based physical sensors have been used in a wide for future researchers. Many research articles are found that
range of skin-mountable and wearable sensor types, with appli- discuss graphene-based wearable sensors and their application
cations ranging from human motion detection to health moni- in different industries. This review particularly focuses on
toring to human-machine interfaces.[27] Figure 1 demonstrates a recent significant research and demonstrates an overall view
summary of graphene-based sensors for various activities, such regarding the utilization of graphene-based wearable sensors
as monitoring some important biophysical, biochemical, and en- in healthcare. The emphasis on crucial applications of the

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sensors along with the fabrication parts makes this review 2.2. Paper-Based Wearable Sensor
more unique and novel than the other published papers to
date. Furthermore, the paper concludes with an illustration of Manufacturing cost is one of the most crucial factors in making
potential future research scopes on graphene-based wearable wearable sensors. In addition to production costs, factors such
sensors in healthcare that will help researchers advance wear- as flexibility, substrate degradation, and process complexity also
able devices for the well-being of humankind and the animal exert influence. Paper-based sensors are getting more attention
world. from researchers due to their multiple unique properties. Primar-
ily, the cost of making them is comparatively low for paper-based
wearable sensors. Besides, paper-based sensors have flexibility,
2. Wearable Sensors in Healthcare Sector are lightweight, and are available in raw materials. One notable
feature of these sensors is their recyclability and biodegradability,
The current healthcare sector in the world is blessed with differ- making them increasingly favored in the context of sustainability
ent types of wearable sensors.[35] The constituent components of and the circular economy. However, there are some drawbacks to
a wearable sensor determine its functionality, mechanical, and these sensors. For instance, paper is inherently insulative; thus,
physical properties.[36] Nanotechnologies, conductive polymers, it is needed to make it conductive through different complex
and 3D-structured materials are mostly preferred to manufacture processes.[44] In addition, wrinkles are another problem with pa-
wearable sensors.[37] Textiles have gained significant prominence per that can result in reduced service life as well as different
as a substrate material in the fabrication of wearable sensors be- sensing errors. Also, a wet environment like underwater is not
cause of their notable attributes of being lightweight and flexible. suitable for paper-based sensors, as paper easily degrades with
These qualities are deemed crucial to meeting the primary needs the touch of water.[10] However, Liu et al.[45] fabricated a superhy-
of wearable sensors.[38] Based on the fabrication material, there drophobic paper-based strain sensor that successfully overcame
are many wearable sensors that are used for multifunctional ap- the wetting property of the paper-based sensor. Scorpion and lo-
plications. The most researched wearable sensors in healthcare tus leaf were utilized to make this water-repellent and highly sen-
are discussed in this section of this review. Table 1 demonstrates sitive paper-based strain sensor (Figure 2b). The coupling bion-
and summarizes different wearable sensors with their properties ics strategy was used to manufacture this sensor, which enabled
and applications. it to monitor real-time human motion as a regular wearable elec-
tronic in all environmental conditions, even underwater. In gen-
eral, paper-based sensors may encounter many limitations that
2.1. Textile-Based Wearable Sensors researchers are actively attempting to address. Nevertheless, their
cost-effective manufacturing process makes them a viable option
Textiles have highly flexible properties, such as being stretchable, for large-scale production,[10] and their biodegradable properties
compressible, twistable, and deformable. In addition to these fea- enhance their superiority over other wearable sensors.
tures, textiles also have other unique properties that make them
a great carrier and substrate for wearable electronics, includ-
ing breathability, lightweight, and high integration with other 2.3. Hydrogel-Based Wearable Sensor
materials.[39] Electronic textiles are one of the most researched
areas that enable wearable sensors to achieve different properties Hydrogel is a three-dimensional porous networked structure
like easy integration with clothing, superior flexibility, and good made of different hydrophilic polymers, such as polyvinyl alco-
abrasion resistance.[10] Also, the lightness and deformation hol, polyacrylamide, etc.[46] One of the unique properties of the
resistance properties of the textile-based sensor made it more hydrogel is that it can retain water up to 99%, which is more
suitable as a wearable sensor.[40] Especially textile-based pressure than human tissue (≈70%).[47] In addition, hydrogels are bio-
sensors are performing very well in different sectors, such as compatible and electric conductive, as well as having distinct me-
medical diagnostics, health monitoring, motion detection, and chanical properties like less elastic modulus, excellent stretch-
home care.[41] Along with the sensibility and detectability prop- ability, and outstanding tuneability that make them an appro-
erties of the sensor, the flexibility, comfortability, and durability priate alternative for the traditional sensor fabrication material
of the sensor should also be considered.[42] Textile-based sensors like an elastomer. Besides, hydrogel, with its excellent mechan-
can exhibit and maintain these properties effectively. Promphet ical features, can properly imitate human skin properties like
et al.[43] designed and fabricated a modified cotton thread col- self-healing; thus, it is an appropriate material for manufactur-
orimetric sensor that can effectively and simultaneously detect ing long-term wearable sensors with intact functionality. Wang
urea and glucose in the sweat of the human body. A mix of et al.[48] developed a wearable strain sensor capable of sensing
chitosan graphene oxide and cellulose nanofiber was used to real-time sweat quantity by using the remarkable water reten-
chemically treat the cotton thread. This made it better at immo- tion capability of hydrogel materials. A super absorbent hydro-
bilizing enzymes (Figure 2a), which means it could be picked gel, consisting of polyacrylic acid and polyvinyl alcohol, was uti-
up by sensors more easily. Due to the flexibility of the cotton lized in this study. This hydrogel has the ability to swell upon
thread, this sensor can easily integrate with the apparel and contact with sweat, hence activating the strain-sensing fabrics.
accessories, which enables it to monitor and regulate glucose These fabrics were created by covering them with conductive car-
and urea levels in the sweat of the wearer’s body. As a result, bon ink (Figure 3a). Figure 3b–d shows the schematic diagram
diabetes and kidney disease can easily be monitored by this of the superabsorbent hydrogel and the workflow of the sweat
sensor. volume monitoring method. This sensor can perfectly measure

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Table 1. Different wearable sensors with their properties.

Wearable Sensor Starting materials Properties Evaluation References

type

Optical pH control and textile wearables Sweat as a sample and textile-based sensing Calorimetric and pH [64]
range
Optical pH-controlled lactate and cotton fabric Sweat as a sample and set on the body Calorimetric analysis [65]
Triboelectric PVDF/Ag NWs- integrated conductive fabric Better air permeability and flexible – [66]
Triboelectric Porous rubber-based carbon fabric Electricity generation with horizontal and – [67]
vertical friction and better durability
Optical Ammonia, Hydrogen chloride, and treated Air as the sample is tested Image analysis [68]
cotton fabric with chemical sensing
electrode
Electrochemical Lactate and woven electrode Sweat is taken for a sample and set on the Amperometric analysis [69]
body
Electrochemical Cotton fabric and sensor Blood leakage monitoring sensor and set on Impedance [70]
the body
Piezoresistive MXene-coated cotton fabric Simple and cheap – [71]
Capacitive SS/PP blended conductive yarn Bi-directional sensing – [72]
Electrochemical Nitro-aromatic explosives and screen-printed Air was taken as a sample Volumetric analysis [73]
electrodes on the textile substrate
Electrochemical NADH, H2 O2 , and screen-printed electrode Sweat and saliva were used as samples, and a Amperometric analysis [74]
on underwear sensor was set on the body
Piezoelectric GO-P(VDF-TrFE)-based fiber membrane Thermally stable and pressure-sensing ability – [75]
Triboelectric Stainless steel fiber-twisted polyester yarn Durable and washable – [76]
Electrochemical Metal ions with controlled pH and textile A complete textile-based sensor Potentiometric analysis [77]
materials
Electrochemical Band-aid, conductive yarn, and polymer Sweat-based analysis and set-up on the body Potentiometric analysis [78]
membrane
Electrochemical Bandages and screen-printed pH-detecting Sweat-based analysis and set-up on the body Potentiometric analysis [79]
sensors
Capacitive GO-doped PU nanofibers and Ni-coated Cheap, weave able, and flexible – [80]
cotton yarn composite yarn
Piezoelectric PEDOT involves nylon fabric Large area capacitive sensor – [81]
Electrochemical Sodium and potassium ions and a Sweat-based analysis and set-up on the body Potentiometric analysis [82]
screen-printed sensor
Electrochemical Glucose/lactate and polyester shirt Sweat-based analysis and setup on the body. Amperometric analysis [83]
Electrochemical Uric acid and bandage with wireless sensor Set-up on the body and sweat as a sample Amperometric analysis [84]
Electrochemical Volatile amine and nano-polymeric It is set close to the body and takes the body Conductometric analysis [85]
composites odor as a sample
Silver and Polymer-coated fabrics Interleukin-6 was used as an analyte, and Stochastic microsensors [86]
carbon-based blood was used as a sample.
polymers
Sodium Ion Carbon fiber-integrated garments Sweat was used as a sample, and the sensor Potentiometric analysis [87]
was used on the body
Electrochemical Polyamide substrates Influenza A virus as an analyte, and it was a Potentiometric analysis [88]
screen-printed sensor
Electrochemical Polymer-coated nylon, NH3 , and DMP Air for the sample was used, and selectivity Conductometric analysis [89]
and sensitivity were introduced for
chemical sensing
Piezoresistive Ni coating on cotton yarn and Skin-integrated devices – [90]
CNT-embedded PU nanofiber-based
composite yarn
Electrochemical NH3 , HCl, and PPy-coated fabric High stability for gas sensing Conductometric analysis [91]
Electrochemical Solvent vapors with carbon black and gas The functionality of an electronic nose Conductometric analysis [92]
sensor integrated fabric
(Continued)

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Table 1. (Continued)

Wearable Sensor Starting materials Properties Evaluation References

type

Electrochemical Polyaniline and NH3 Commercial yarns are used, and air samples Conductometric analysis [83]
are used
Piezoresistive AuNPC-MoS2 coating on the composite fiber Flexible and washable – [93]
Piezoelectric ZnO and conductive woven fabric Optimizable sensor and pressure range with – [94]
high sensitivity
Gas sensor rGO and nanomaterials Machine learning-enabled and IoT-based Calorimetric analysis [95]
graphene gas sensing

the volume of sweat by changing the resistivity of the strain- Classic sensors have a lot of problems, like being expensive, not
sensing fabrics, which was further displayed on the monitor.[48] being biocompatible, having rigid substrate materials, being hard
However, hydrogel is still facing some drawbacks that need to be to make, and not being able to sense strain. Graphene presents
addressed to be a suitable constituent material for wearable sen- a potential remedy for the aforementioned limitations owing to
sors. For example, the weakening of hydrogel adherence to the its cost-effectiveness, heightened sensitivity, and expansive oper-
electrode during electrochemical performance owing to swelling ational scope, among other attributes.[49] Graphene has excellent
and shrinking is a serious barrier to long-term application with electron mobility, thermal conductivity, and flexibility; as a re-
good functionality.[10] sult, various mechanical sensors can easily be obtained from it,
such as breath, sound, pulse, human motion, etc. The excellent
2.4. Graphene-Based Wearable Sensor performance of graphene as a chemical sensor is a result of its
large specific surface area and ultralight properties.[22] Overall,
Graphene is one of the most suitable fabrication materials for graphene is an excellent candidate for the fabrication of wearable
wearable sensors due to its multiple excellent characteristics. sensors due to its excellent sensing, mechanical, optical, thermal,

Figure 2. a) Schematic fabrication process of a modified cotton thread colorimetric sensor developed by Promphet et al. Adapted with permission.[43]
Copyright 2023, Elsevier Limited. b) The schematic manufacturing and design concept of a strain sensor based on superhydrophobic paper and SEM
analysis of the surface morphology of a scorpion’s slit unit and a papilla (lotus leaf). Adapted with permission.[45] Copyright 2021, American Chemical
Society.

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Figure 3. a) Image of the strain-sensing fabric b) sweat-absorbing hydrogel; dry hydrogel absorbs sweat and swelling till final equilibrium (left to right); c)
cross-section view of hydrogel-attached sweat gland; d) hydrogel’s response to sweat along with real-time signal monitoring. Adapted with permission.[48]
Copyright 2023, Elsevier Limited.

and electrical properties.[10,50] Graphene-based wearable sensors et al.[54] prepared a wearable sweat capture sensor by utilizing pat-
can be of various types based on their functions and properties, terned graphene arrays. The patterned graphene arrays were su-
such as mechanical sensors[49a,51] (i.e., human motion, pulse, and per hydrophilic and showed strong bonding to capture droplets of
breath), fluid sensors,[52] acoustic sensors,[53] electrophysiolog- sweat even in modest physical exercise. Figure 4c shows the sweat
ical sensors,[54] and gas sensors.[55] In the case of a graphene- capture band that was made with patterned graphene arrays on a
based mechanical sensor, accurate detection of the mechanical pristine polyimide substrate. The strong attachment between the
signal is required within a small range of strain or pressure, such water droplets (sweat) and the patterned graphene arrays in the
as heart rate.[49a,56] Yang et al.[57] prepared a polyester fabric-based band’s positions of upward, downward, and sideward is demon-
graphene mechanical sensor that can detect both large and small strated in Figure 4d–f.[54]
human body motions. Very small signals like diastolic waves,
percussion waves, and tidal waves can be effectively detected by
this excellent wearable sensor. This sensor can detect not only 3. Fabrication Methods
the subtle signals of the human body but also significant move- Graphene should have been structured into different patterns
ments such as the bending of the knee, wrist, elbow, and fin- to fabricate functional devices. As a result, numerous strategies
ger. Figure 4a,b shows the attachment of this sensor to different have been proposed.[26] The method used to synthesize graphene
parts of the body for sensing small and large motions. Due to has a significant influence on the patterning method utilized.
its excellent thermoacoustic and piezoresistive effects, graphene Moreover, resolution, cost, and substrate are all important factors
is also being extensively researched for sound sensing[58] and to consider when selecting a patterning method.[22] This section
for sound emission.[59] Graphene-based wearable acoustics sen- briefly describes various patterning approaches used in the fabri-
sors are superior in many ways, such as graphene sensors have cation of graphene devices. Figure 5 summarizes all the fabrica-
lower fluctuations and a wider range of frequency.[60] Addition- tion methods, including different printing techniques for sensor
ally, all kinds of graphene, including multilayer or single-layer, development
can be utilized in acoustic applications.[22] On the other hand,
for measuring bioelectricity, the traditional method used wet elec-
trodes placed on the human body.[61] However, it has been found 3.1. Photolithography and Plasma Etching
that wet electrodes are not good for human skin as their con-
stituents can maintain good attachment with the human body Photolithography is a widely employed form of lithography pro-
even during exercise and home care. In the case of dry electrodes, jection that involves the selective exposure of a photosensitive
graphene performs wonderfully due to its super flexibility and polymer to light through a mask. The objective is to generate a
good conductivity.[22] Thus, graphene-based wearable sensors are desired image in a nano-polymer, thereby creating a patterned
widely researched for electrophysiological signal sensing, like entrance to the elementary polymer.[96] Figure 5a depicts the
ECG,[62] EOG,[63] EEG,[62c] and EMG.[62c] Graphene-based wear- photolithography and plasma etching processes. Plasma etching
able sensors also work well in body fluid sensing like glucose, is the process of removing unwanted material from a treated
sweat, etc., and different gas sensing. The large specific surface surface by using plasma with overlay accuracy. Photolithogra-
area of graphene helps excellently in gas and fluid sensing.[22] Li phy is expected to be an effective process for graphene due

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Figure 4. Schematic of the sensor attachment for detecting a) subtle motion and b) large movement of the human body.Adapted with permission.[57]
Copyright 2018, American Chemical Society. Digital image of a wristband wearable sweat capture sensor; c) water captured by the wearable sweat capture
sensor when the sensor is d) upward, e) sideward, f) downward. Adapted with permission.[54] Copyright 2019, American Chemical Society.

to its smooth surface and exceptionally low thickness.[97] Yang tion of graphene to its initial phase.[102] After a few years, in 2017,
et al.[98] fabricated graphene-based and flexible NO2 sensors on it was found that cyclic etching (two-step plasma etching pro-
paper that could generate faster responses (nearly ≈32–39%). cess) can prevent the graphene surface from being destroyed.[103]
They used 200 ppm of NO2 gas with a strain of 0.5%. More- The benefits of using the plasma etching process include im-
over, after forming two electrodes with Ag pastes, they used a proved surface treatment, removal of metal-coated substrates de-
poly (methyl methacrylate) layer for transferring the graphene spite their strong adhesion to the surface,[104] precise control of
fabricated in the chemical vapor deposition process. For better multilayer graphene, thickness uniformity without causing sur-
evaluation, they evaluated their current-voltage dynamic sensing face changes, and suitability for nano-electronic devices based on
performance in both strained and relaxed situations. Most im- two-dimensional (2D) materials.[103] The high price of the per-
portantly, they demonstrated photolithography with a higher vac- manent mask and the inability to treat honeycomb graphene’s
uum process for fabricating graphene sensors with higher perfor- extremely rough surface are two of the process’s drawbacks.[97]
mance. Next, Wang et al.[99] developed micro-patterned sensors
over skins for monitoring human physiological signals by pho-
tolithography process for strain sensing. Their fabricated wear- 3.2. Laser Scribed Graphene
able membrane-based sensors could separately manage physio-
logical parameters and different physical activities, like athletic Laser-scribed graphene (LIG) is one of those fabrication pro-
movements. Various etching methods are used for graphene, cesses that use a programmed procedure for patterning rather
but O2 plasma etching is considered to be the best option for than a mask (Figure 5b).[97] A mobile and disposable non-
patterning.[97] In 2011, the use of nanosphere lithography with enzymatic glucose sensor strip, initially based on gold nanopar-
low-power O2 plasma proved to be a good choice for locating ticles, was developed after modifying laser-scribed graphene,
various branches, chains, and connected circular rings.[100] An- and it was a cost-effective way for applications such as glucose
other procedure for thinning graphene in a layer-by-layer way was level self-monitoring and nutrition management.[105] Wearable
established using mild N2 plasma along with post-annealing in energy storage electronics seek to be mechanically conformable
Ar/O2 .[101] The O2 plasma approach was favored despite being for optimal comfort, adaptability, and thermal stability. There-
more effective due to the formation of defects on the surface of fore, there is a lot of research going into creating supercapacitors
the graphene lattice.[101] Graphene hydrogenation by ion-etching (SCs) as a replacement for microbatteries in microelectronics.
plasma was developed in 2011 and could reverse the hydrogena- Using a laser-induced graphene-based flexible interdigital elec-

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Figure 5. Various patterning methods for graphene-based wearable sensor development a) Photolithography and plasma etching process of
graphene,[126] b) Illustration of the laser-scribed graphene process,[127] c) Transfer printing process,[127] d) Illustration of inkjet printing technique,[127]
and e) Graphene hard mask patterning technique.[128]

trode, Awasthi et al.[106] created a tiny supercapacitor that is stable 3.3. Transfer Printing
throughout a wide temperature range. A flexible laser-induced
graphene (LIG) supercapacitor electrode fabrication method us- Transfer printing is an excellent choice for applications such as
ing a CO2 laser was introduced in the study. EDX spectroscopy transistors and energy storage where patterns with extremely
and scanning electron microscopy both validated the morphol- high, clear, and precise resolution are required.[97] It can be a
ogy and development of LIGs. Charge-discharge cycles, capac- positive or negative pattern transfer depending on the extrac-
itive performance, power density, and cyclic life were all im- tion or repositioning of materials between layers of substrate and
proved with interdigital LIG electrodes designed specifically for mask, as shown in Figure 5c. As a transfer stamp, the gold film
supercapacitors on a flexible substrate. The 3D porous LIG su- was used for transferring the pattern of graphene, and this tech-
percapacitor, made possible by an optimized PVA-KOH gel elec- nique was suitable for applying to any substrate over large ar-
trolyte, has an areal capacitance of 83.33 mF cm−2 at 0.5 mA eas, which paved the way for its use in electrical applications.[108]
cm−2 current density, 4.62 Wh cm−2 at the same current density, Later on, by using the soft transfer printing method, ultra-large
and a power density of 0.2 mW cm−2 at the same current den- graphene oxide sheets (up to 100 micrometers) were transferred
sity. One possible benefit of this method is that it can do both onto PET substrates, which was proven to be a cheap, melodi-
growth and pattern formation at the same time, thanks to a pro- ous, efficient reduction process and also a promising technique
grammable process that gets rid of the need for a mask. Addition- to produce flexible TCFs as well.[109] Oren et al.[110] reported a
ally, this method offers a time-saving advantage and allows for facile way to pattern graphene sensors by transferring the print-
the possibility of grooving the pattern on a carbon source sub- ing process with drop-casting of graphene film from a prepat-
sequent to its capture by a laser platform.[97] This method has terned polydimethylsiloxane (PDMS) membrane to the target
the limitation of producing a sloppy pattern with poor resolu- tape. The micrometer-sized graphene was transferred on the final
tion. In terms of commercialization, laser scribing technology al- tape, and this process was quite easy to implement and did not
lows for rapid, large-scale, and low-cost production of the LSG, require any heavy equipment for the patterning process. Trans-
which is a significant advantage in the development of pressure fer of chemical vapor deposition graphene to an assigned 3D
sensors.[107] molecular surface was possible by applying the water transfer

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printing method, which had the advantages of using uncompli- and lifting off, which are indifferent to photolithography.[97] The
cated tools, operating at room temperature, and ingesting low only difference is that the photolithography process has a trans-
amounts of reagents.[111] The transfer printing method can also fer pattern, and the hard mask process uses a hollow pattern
be combined with other methods such as holographic lithogra- (Figure 5e).[97] The process can be combined with other meth-
phy, plasma etching,[112] laser scribing method.[113] This method ods, such as lithography, for defining graphene patterns.[123] As a
has a number of benefits: it is easy to set up, it works well flexible power source, the printed finger structure can be applied
for large-scale industrial applications,[114] it has a technique that to a micro-supercapacitor array and integrated with a flexible
can be used by other people, it has a high and accurate pattern strain sensor. Xiong et al.[124] created a patterned GO/polyaniline
resolution,[97,115] and it allows for separate assembly and device (PANI) gel by combining spraying and the hard mask. The ad-
component fabrication.[116] The disadvantages include the high vantages of this method include a confrontation with proximity
costs brought on by using fixed masks and the high interface effects and the ability to control lift-off reliability with the hard
requirements.[97] The most common screen-printing mask is a mask method. Additionally, underexposure to the honeycomb
stainless-steel sheet scribed with a laser. Secor et al. combined pattern results in an increase in the process window and im-
screen printing and transfer printing to create the gravure print- proved resolution.[125] The disadvantages include increased ex-
ing of graphene.[117] The development of appropriate inks and penses due to the need for masks and the requirement for more
printing parameters allows for the fabrication of patterns with time.
resolutions as low as 30 μm.

3.6. 3D Printing
3.4. Inkjet Printing
The fabrication of graphene-based wearables via 3D printing is a
Inkjet printing, which uses a programmable controller instead fascinating convergence of modern materials and manufactur-
of a mask to realize patterning, has been one of the most de- ing technology, giving a variety of new possibilities for devel-
manding fabrication techniques over the years.[97] As the mate- oping useful, flexible, and high-performance wearable devices.
rial passes through the print head, nozzles in the head spray ink Graphene, a one-atom-thick sheet of carbon, is well known for
onto the material (Figure 5d). Graphene inks are typically pre- its superior electrical, mechanical, and thermal properties, mak-
pared using liquid-phase exfoliation.[118] Silver, gold, graphene, ing it an excellent option for usage in wearables.[129] 3D-printed
and carbon nanomaterials are the primary components of inkjet- graphene wearables have been used for a variety of reasons in
printed conducting materials.[119] A water-based inkjet printable healthcare. They can, for example, be used to continuously mon-
ink was created using electrochemically exfoliated graphene, and itor vital signs such as heart rate, body temperature, and respi-
it was found to have greater sheet resistance than any other ink ration rate. Furthermore, graphene-based sensors can be pro-
produced by LPE.[118] Another fabrication technique was used on grammed to detect specific biomarkers in human fluids, en-
photographic paper for the application of a fully inkjet-printed abling early illness detection and tailored health monitoring.[22]
gas sensor matrix, which demonstrated excellent stability and The initial stage in making graphene-based wearable sen-
flexibility under various bending and long-term dynamic sens- sors for healthcare applications is to make graphene-based ink.
ing tests.[120] Other amazing works on inkjet printing include Graphene flakes or nanoplatelets are dispersed in a suitable sol-
the combination of inkjet printing for healthcare and wearable vent to create this ink. To attain the correct ink viscosity for com-
devices,[121] the development of stretchable graphene conductors patibility with 3D printing procedures, the solvent and graphene
for wearable technology,[122] and so on. Wearable sweat sensors content in the ink must be carefully determined.[130] After the
have the potential to advance precision medicine by collecting graphene ink and substrate have been created, the 3D printer
health-related molecular data in a non-invasive manner. Unfor- must be set up for printing. To ensure compatibility with the
tunately, it is still difficult to continually detect several critical graphene ink, printer settings must be adjusted, including noz-
biomarkers with existing wearables. The benefits of inkjet print- zle size, temperature, and layer thickness, among other charac-
ing include low-cost changes in printed design due to the lack of a teristics. To obtain the desired precision in printing, proper align-
mask, ease of development,[119] non-contact manufacturing tech- ment and calibration are required.[130] The 3D printer must be
niques, and essential sensing capabilities. Disadvantages include adjusted for printing after the graphene ink and substrate have
the need for more time for ink preparation in order to achieve been created. It is critical to adapt the printer settings to ensure
high concentration,[118] and low resolution.[97] compatibility with the graphene ink, which includes considera-
tions for nozzle size, temperature, and layer thickness, among
other characteristics.[129] Proper alignment and calibration are re-
3.5. Hard Mask quired to obtain the requisite precision in printing.[22] Following
the printing procedure, the graphene ink on the substrate must
The hard mask technique, which uses a hollow pattern for the dry and cure. This is usually accomplished through a combina-
materials being passed through and has numerous applications, tion of thermal and chemical treatments. The curing procedure
has been used for several years. After placing a hard mask on is critical for maintaining proper adhesion between the graphene
the surface, graphene ink is dropped, and any excess ink is dis- and the substrate as well as improving the printed sensor’s elec-
carded into hollow parts. After the ink has dried, the mask’s hol- trical conductivity.[130]
low shapes are turned into graphene patterns on the substrate. 3D bioprinting with different functional 2D materials has
There are two methods for the hard mask of graphene: etching added a different dimension as a present-day technology. It

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Figure 6. Graphene-based 3D printing fabrication techniques and applications.

is also considered a part of additive manufacturing, which have an ensured cursive deposition with very few defects. At the
shows ground-breaking potential in modeling and remodeling beginning of the world of 3D printing, Das et al.[136] considered
approaches in healthcare applications. It can generate living tis- mechanical flexibility as a core issue in the use of graphene in
sues from the tissues of the mother cell, and it can provide differ- electronics and wearables. They considered the fast fabrication of
ent and highly accurate biological signals with biosensors made ink-jet-printed graphene circuits at a cheaper cost and in a sus-
with materials like graphene or other 2D materials. Because of tainable way. Therefore, this non-toxic agent can process ink that
this, graphene can be combined with the 3D bioprinting method can be used in conductive stripes on different flexible wearables.
and the ideas behind biomimetic acts.[131] Figure 6 demonstrates Using a powdered bed with graphene with injection molding and
different aspects of incorporating graphene in 3D printing and binder in the feed is not a bad idea at all. Azhari et al.[137] intro-
its applications. Bio-fabrication processes in human organs or duced the process of fabricating quasi-ink, and they could develop
tissues may happen in three ways: pre-bioprinting, 3D bioprint- some regular slices of the sensing materials. Moreover, this pro-
ing, and post-bioprinting. The entire process includes selecting cess can easily be incorporated into different sensing applications
the materials and appropriate processing techniques, evaluat- like immunodetection and therapeutics. When the problem was
ing the material flow, and finally getting through to the applica- about the cost and processing time of sensor fabrication with 3D
tion stage.[132] Additionally, mature constructs are cultured in the printed sensors, Davoodi et al.[138] used dip coating with porous
post-printing period in a substantial environment that is almost polymers with graphene to fabricate conductive layers integrated
close to the native environment of the cell.[132,133] into the silicone sensors that are ordered and interconnected to
People all over the world have suffered a lot and faced a dev- each other. The 3D-printed mold was dip-coated into the silicone
asting state in healthcare due to COVID-19 during the 2020 rubber surface, and with a stable coating, the sensors had sta-
pandemic.[134] The situation was quite out of hand due to the ble electric conductivity for ≈ 12 months. This sensor can easily
spread and growth of infectious diseases. 3D printing technolo- take signals from human movement, small deformations like a
gies with graphene have the ability to fight against infectious human pulse, and many more.
diseases, and they perform so efficiently as vaccines, therapeu- Though graphene inks are quite capable of having some ab-
tic agents, and in vitro modeling.[135] Graphene-based inks are stract properties to endow superior functionalities, there are
also used in 3D-printing constructs for different biosensors and some parts to consider in processing them for 3D printing, espe-
wearable sensors, with diverse scopes for applications. To fabri- cially in healthcare applications.[129] For example, the ink and its
cate a 3D structure through printing with an appropriate rheo- fabrication need to be in accordance with user and eco-friendly
logical property, the friction efficiency in the system should be procedures and environmental factors, and the variations must
maintained as low as possible; hence, the obtained construct will be evaluated strictly. The best-fitting printing technique for the

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Table 2. A comparison of various graphene patterning techniques.

Fabrication techniques Cost Programmable Advantages Disadvantages

Photolithography and High No Better surface treatment, removal of metal-coated High cost, presence of an unchangeable mask,
plasma etching substrates,[ 104] precise control, thickness uniformity, and not being able to treat honeycombed
suitability for nano-electronic devices based on 2D graphene with an extremely bristle surface[ 97]
materials[ 103]
Hard mask Medium No Confrontation with proximity effects and lift-off reliability More cost, use of masks, and requirement of
can be controlled. Underexposure to the honeycomb more time.
pattern, increment of the process window, and better
resolution[ 125]
Transfer Printing High No Simple equipment, beneficial for industrial-scale High cost, presence of an unchangeable mask,
applications,[ 114] has transferrable technique, high and demand of high interface[ 97]
precise resolution of pattern,[ 97,115] and enables
distinct operation of assembly and device component
fabrication[ 116]
Inkjet Printing Low Yes Changes in printed design with low cost, no use of masks, Requirement of more time for ink preparation in
ease of development,[ 119] non-contact manufacturing order to achieve high concentration,[ 118] low
techniques, essential sensing capabilities resolution[ 97]
3D printing High Yes It can make prototypes rapidly, and it can be modified It requires highly skilled manpower and a slower
faster. It can generate complex 3D structures fabrication process, and there has been a
scarcity of materials
Laser Scribed Graphene Low Yes Growth and pattern in one step, programmable Low-resolution pattern
procedure, no use of mask, less time-consuming,
possibility of pattern being grooved on a carbon source
after taking output pattern on a laser platform.[ 97]

best precursor should be fixed beforehand to get the best output non-destructive human monitoring device, Chen et al.[140] were
from the process.[132] Researchers are working more on develop- finally successful in developing a specific approach to a pressure
ing more tunable and geometrically controllable sensing materi- sensor with 3D microstructures in 2019, using the extremely use-
als with graphene in the wearable sector.[22] ful properties of graphene. The path was not that easy for them,
Table 2 summarizes all the features and attributes of differ- as the pulse and the blood vessels are just beneath the skin, and
ent fabrication techniques for graphene-based wearable sensors. thus the very delicate and tiny signals are tough to detect. An in-
Furthermore, the table summarizes the advantages and disad- terfacial self-assembled graphene film, or ISG, has been devel-
vantages of different fabrication techniques and gives a relative oped in ultra-large form via self-assembly and an environmen-
idea of the cost of production. Correspondingly, different sensing tally friendly process, and this structure produces some brilliant
applications with graphene-based wearables in healthcare have outputs for ready-made 3D sensors, particularly with excellent
been demonstrated in the following section of this review. sensitivity in the detection of the pulse rate as well as the mo-
tion since the wrist was bent. In addition to that, this innovation
has aggrandized the research in graphene a lot as it provides a
4. Graphene in Wearable Sensors For Healthcare novel, superior, and tunable sensitivity within the range of 1.04
Applications to 1875.5 kPa−1 since the range of detection has ranged from 1 to
40 kPa.[141]
Graphene’s exceptional properties of high thermal conductivity, Evaluating and monitoring the human body’s locomotion has
superior electron mobility, and a large surface area with limited been an important part of quantifying human health conditions
thickness have propelled it to a point where a wide range of appli- and performance, as well as providing patients with care when
cations are now readily available. All of this is possible because they are not in the hospital.[29] Furthermore, graphene-based
the properties are fortunately concentrated in a single material, wearable sensors have enormous potential for biomedical appli-
graphene.[97] There are several applications of graphene, and cations and human motion monitoring. Musculoskeletal func-
this section discusses the application of graphene-based wearable tions and human gait are important kinetic parameters in games
sensors. Figure 7 illustrates different healthcare applications of and sports in terms of quantitative evaluation, and they also have
graphene-based wearables. a great impact on the detection and running diagnosis of vari-
ous diseases prior to cardiopathies, aging, dementia, and some
other neurodegenerative disorders like Parkinson’s and other
4.1. Human Movement, Gesture, And Health Monitoring sclerosis.[142]
Extensive research has been conducted on textile sensors
The 3D graphene sensors are pretty amenable to application in designed for application in wearable monitoring. The sensor
terms of human health detection as well as monitoring from time systems require a large sensing area, adaptability, and a man-
to time.[139] After numerous efforts by researchers to develop a ufacturing process that can be scaled up. Choudhry et al.[143]

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Figure 7. Graphene-based wearable sensors in healthcare applications.

fabricated textile-based flexible pressure sensors using a single make it easier and more convenient.[144] Zhang et al.[145] fabri-
layer of material for use in smart wearable electronics. Using con- cated a graphene-coated fiber sensor with superior sensitivity and
ductive threads and fabrics covered with metallic and graphene high reproducibility in terms of performance. They attached the
nanoplatelets, single-layer piezoresistive sensors were created sensors to several parts of the body of the athletes, including the
using a machine stitching process. Because the area of contact shoulder, elbow, wrist, knee, and ankle, to capture the motion of
between the conductive thread and fabric altered in response to the human body. As a result of analyzing the raw data, they were
pressure, these sensors worked. The single-layer construction able to obtain precise monitoring of the motion.
ensured flexibility, reducing physical drift caused by human There is a growing interest in graphene-based aerogel/spacer
activity and boosting both comfort and efficiency. Scanning elec- fabric composites for use in healthcare, notably in sensing. These
tron microscopy and Fourier transform infrared spectroscopy composites, based on the porous structure of aerogels and the
were used to characterize coated fabrics. Wearability and sensing amazing characteristics of graphene, provide a viable platform for
capability were validated via extensive physical and electrome- healthcare sensors. They are perfect for building sensors for med-
chanical testing, with the sensors demonstrating a 100 kPa ical monitoring, diagnostics, and individualized healthcare due
working range, extraordinary sensitivity, and resistance to me- to their lightweight, extremely porous structure and graphene’s
chanical deformations. The successful integration of sensors into superior electrical and mechanical characteristics. For this better
garments for real-time monitoring and posture correction has sensing prospect and potential with protection, Wang et al.[146]
proved their potential as durable, adaptable, and highly effective created wearable multifunctional graphene-based aerogel/spacer
pressure sensors suitable for smart wearable applications. fabric composites. A flexible composite material was created by
The sensors can monitor the high-risk patient’s actions over combining the mechanical qualities of the spacer fabric with the
time using wearable sensors since there is an assistive tool es- electrical features of graphene-based aerogels. A 1.48 strain sensi-
tablished in the body to obtain information from asymptomatic tivity, a temperature of −0.004 °C in the sensitivity, and a 45 per-
individuals and patients. The most often employed and accessible cent protection factor were all displayed. This ultra-thin, water-
sensors for gait analysis include inertial sensors, optical sensors, repellent, thermally insulating material worked well through-
and angular sensors. However, the inertial sensors include multi- out a wide temperature range, from ≈ 180 °C down to much
ple sensor combinations among the accelerometers, gyroscopes, lower temperatures. Previous studies indicated that the multi-
and magnetometers. The inertial sensors function mostly based functional composite could be useful not only as a building ma-
on Newton’s third law, and they are set to the inertial measure- terial but also as an intelligent cushion in the medical field.
ment unit of the body (IMU). Moreover, multiple sensors are in- Interactive wearable sensors have become so prevalent that
tegrated into it, and thus the generated signals drive the IMU to the need for flexible electronics and devices has been skyrocket-
measure angular velocity, angle of flexion, 3D linear acceleration, ing in healthcare. Larimi et al.[147] fabricated an inexpensive and
and coordination with the reference frame. The below and above stretchable strain sensor for monitoring the motion of the human
joints are the best places to fix the rigid small IMU, i.e., the knee, body and organs using bio-signals (Figure 8a). They introduced
hip, elbow, toe, shoulder, neck, and ankle are the places where the piezo-resistive sensor for measuring a wide range of human
it can monitor the walking speed, condition, joint movement, motion. This highly stretchable graphene-based sensor can keep
and running conditions. However, the IMU is the most perfect the strain withstand able to a significant extent (up to 350%). It
method for clinical gait analysis. The integration of graphene can sustains itself even after 10000 cycles of strain. Moreover, this

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Figure 8. Graphene-based wearable sensors in human motion monitoring a) preparation of GNF-pad by infusing the graphene nanopowder into a clear
adhesive pad. Adapted with permission.[147] Copyright 2023, Elsevier Limited. b) a biocompatible strain sensor with conductive polymers. Adapted under
the term of Creative Commons Attribution License 4.0 (CC BY).[148] Copyright 2021, The Authors, published by Licensee MDPI.

sensor also works fine in robotic fingers with real-time monitor- swallowing, opening of the mouth, speaking, blowing, shouting,
ing of different human interactions. Jiong et al.[148] developed a crying, breathing, and squatting. Its sensitivity was adjustable,
biocompatible strain sensor on elastomeric conductive polymer ranging from 0.042 to 0.152 kPa−1 , and it could detect both large
composites to develop human monitoring devices (Figure 8b). and small movements. Its response time (96 ms), functioning
They used an e-skin substrate with polydimethylsiloxane (PDMS) range (0–27 kPa), and durability (> 9000 cycles) steal the lime-
and a photosensitive polyimide (PSPI) precursor, followed by the light easily.[141,150] Islam et al.[151] fabricated a fully printed and
formation of LIG/PDMS/PSPI composites with the laser direct conductive energy-storing wearable sensor to monitor human
writing (LDW) process. A combination of minimalistic oscilla- movements with different bio-signals (Figure 9a). Highly scal-
tion and physiological signals was generated for intelligent sound able printing for sensor development with graphene ink could
sensing. Moreover, it showed an excellent sensing range (120%), detect different activities of the human body. Moreover, it showed
a higher gauge factor of ≈ 380, and a very short response time of superior aerial capacitance with excellent stability. Additionally,
90 ms. it can monitor brain activities for different electrophysiological
When tiny and strong pressure sensors are available with a signals. Bai et al.[152] developed an inexpensive technique to fab-
wide range of monitoring abilities, a 3D graphene-based wear- ricate graphene-based yarn sensors (GYS) in combination with
able pressure sensor can easily evaluate human motion. Joint graphene oxide (GO) coatings with polyester (PE) and wound
bending is comparatively a robust movement with a value of spandex yarns (Figure 9b). It had the ability to tune the sensitivity
>20 kPa, and the movements generated from speaking and pul- as well as the gauge factor from 0 to 50%. This direct wound yarn
sating cause barely <1 kPa. Therefore, it has been a challenge sensor can essentially monitor different motions in the human
to distinguish the movements and monitor them. Researchers body with muscles in relaxing and contracting conditions.
were trying to find a way to get out of this limitation.[149] Finally, The strain sensors let the device get information from the hu-
Dong et al.[149] came up with a solution. The group has fabri- man body and keep the device and the human body in touch.
cated a 3D rGO/polyaniline sponge (RGPS) for detecting human The thin, hydrophobic, flexible, human-skin-colored sensor has
motion by constructing multi-level microstructures with a feasi- been directly set to the human body, a handicapped prosthetic
ble method. The 3D graphene sponge has a delicate microstruc- limb, or a functioning robot. PDMS was used as a main part of
ture, and its positively charged PANI and negatively charged rGO the strain sensors because it is hydrophobic, easy to shape, has
make it a hybrid sponge. The synergistic impact of it provides low interfacial free energy, and is stable at high temperatures and
a flexible and ultra-light sensor with high sensitivity to monitor chemicals. As a carbon-based material, graphene has attracted

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Figure 9. a) A fully printed graphene-based multifunctional sensor for monitoring human movement. Adapted with permission.[151] Copyright 2022,
Elsevier Limited. b) Stretchable graphene-based thin film-coated yarn sensors for human motion monitoring. Adapted under the term of Creative Com-
mons Attribution License 4.0 (CC BY).[152] Copyright 2019, The Authors, published by Springer Nature.

great attention for its higher thermal conductivity and optical 800% were tolerated by the optimized thermoelectric composite
transparency.[153] 3D porous graphene structures (3-D PGS) can threads. Excellent thermoelectric stability was maintained even
be implanted in so many sensors that they have a great impact after 1000 bending cycles. Using the thermoelectric effect, this
on fabricating a device for human motion monitoring. Laser- technique can measure strain and temperature with extreme pre-
induced graphene can release properties like graphene. So many cision. These thermoelectric threads allowed for the autonomous
researchers have already worked on it.[154] Although ample effort monitoring of physiological signals in wearable devices, such as
has been made in the development of wearable sensors, it still the degree of mouth opening, occlusal frequency, and tooth force
requires a long way of study to make it more pragmatic for pre- when eating. This breakthrough yielded useful information that
cise, long-term, durable, and continuous human monitoring ac- can be used to promote better dental health and healthier diets.
tivities. The efficient form factor, high flexibility, robustness, and As the demand for polymer-based composite strain sensors
efficacy of the final device with respect to energy consumption rose by that time, Sankar et al.[156] developed flexible hydrogen-
are places where it still needs to be improved. It is still challeng- exfoliated graphene (HEG)-based strain sensors with piezoresis-
ing to integrate piezoresistive materials into an apparel product tive action with waterproof poly(vinylidene difluoride) (PVDF) to
with a superior gauge factor and better stretchability up to a sat- get higher conductivity in the sensors used in different wear-
isfactory level. The wearables’ high linearity with low hysteresis ables and human health monitoring devices (Figure 10a). This
behavior, data acquisition, and transmission in human gait mon- PVDF/HEG-based strain sensor exhibited 0.3 S cm−1 of elec-
itoring, comfortability, data breach when processing, and privacy trical conductivity and a maximum gauge factor (GF) of 10,
are still major concerns.[144b] which made the sensor exclusive to the other available devices.
Flexible sensors play a crucial role in the development of in- Some of the cardiovascular difficulties happened in the absence
telligent electrical gadgets. Strain sensing is one of their most of portable and flexible monitoring of real-time health. To re-
important uses and underpins several other technologies. To duce the mortality rate, Chen et al.[157] fabricated a device to de-
usher in the next generation of smart electronics, it is crucial tect physiological signals with a LIG-based E-skin that can mon-
that high-performance flexible strain sensors be developed. For itor the health condition and respond in alarm as an output
autonomous oral health monitoring, Li et al.[155] developed 3D ex- (Figure 10b). Moreover, the sensor showed excellent acoustic and
truded graphene thermoelectric threads. Using graphene-based mechanical performance with higher sensitivity (316.3 units) and
thermoelectric composite threads, researchers created a self- could detect bio-signals related to pulse, respiration activities, and
powered, ultrasensitive strain sensor. Extreme stresses of over many more. Shathi et al.[158] fabricated a smart textile sports bra

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Figure 10. Graphene-based wearable sensors in healthcare a) PVDF/HEG-based strain sensor for human health monitoring. Adapted with
permission.[156] Copyright 2020, American Chemical Society. b) Laser-induced graphene (LIG)-utilized electronic skin (E-skin)-based sensor. Adapted
with permission.[157] Copyright 2023, John Wiley & Sons. c) From cutting the fabric electrodes and setting them in a sports bra: the notion indicates left
straps (L), right straps (R), and bottom rib electrodes (H), and then the performance of the smart textiles was evaluated. Adapted with permission.[158]
Copyright 2023, John Wiley & Sons.

with a coating of graphene that can be used in human health easily distinguish normal and abnormal breathing in the patient
monitoring (Figure 10c). They used the pad-dry-cure method to with very nuanced information, and the ultimate evaluation is
fabricate the electrode, and the electrical performance was signif- visible in the mobile application. Hence, it has made diagnosis
icantly improved. Then, they incorporated rGO into the layer-by- and monitoring very accessible with a facile fabrication process
layer (L-b-L) method. With a highly sensitive response rate, this of simple coating with functional graphene materials.
smart wearable can easily monitor different parts of the human Despite the presence of some necessary cracks, graphene has a
body. significant piezoresistive impact in terms of its flexible mechan-
COVID has taught us a great lesson in the prevention of the ical performance in sensors. Breath rate, heart rate, and pulse
spreading of the virus; hence, facemasks play a very important could be measured with the conventional mechanical signaling
role in resisting virus-containing fluids or air from entering our process, but its accuracy was bound by a short range of pressure
bodies. The virus directly attacks the lungs, which eventually cre- and strain.[49a,56] To provide a solution to that, Yang et al.[57] fab-
ates problems with breathing. In this circumstance, it is impor- ricated a textile sensor with graphene to detect precise and large-
tant to monitor the health status of the patient from time to scale human motion. Aside from accurately capturing pulse sig-
time. However, collecting respiration information from the hu- nals, it could also detect changes in relative resistance during
man body and real-time tracking of the signals are not easy jobs mouth opening and closing, as well as waves such as the tidal
to maintain. Moreover, fast responses and biocompatibility have wave (T-wave), percussion wave (P-wave), and diastolic wave (D-
been issues in wearables for a long time. As a response to the wave). The electronic skin for the epidermal part, with multilay-
above-mentioned issues, Bidsorki et al.[159] developed a wearable ered and laser-scribing graphene, developed by Qiao et al,[160]
and smart face mask with graphene materials that could easily could be able to capture the respiratory signals and could iden-
be used in healthcare for real-time monitoring of human res- tify the levels and conditions of graphene when it has been set to
piration. The smart face masks were fabricated with graphene the throat or mask. A graphene-paper sensor, on the other hand,
nanoplatelets and polycaprolactone (PCL) over normal surgical can detect subtle pressures such as pulse and gas pressure. A
masks in a certain polymeric matrix. With excellent durability strain sensor on woven fabrics, fabricated by Wang et al.[161] by
and >1000 cycles of stability, the face masks exhibited a very fast the CVD method, was quite amenable to defining the physio-
response time of nearly 42 ms during the tests. Moreover, it can logical signals and human-generated micromotions when it was

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fixed to the mouth, and it could detect the change in facial ex- healing push it over the mark in terms of its efficacy. The imple-
pression, the resistive changes, as well as the blinks, and the mentation of 3D graphene drives it even beyond the abovemen-
respires, respectively. Graphene-based wearable sensors can be tioned applications.[141]
used in invasive and non-invasive applications. Moreover, the in- Chun et al.[166] developed a water-resistant e-skin for wearable
vasive applications include the nervous system, cardiovascular fabric sensors using graphene (Figure 10a). Getting inspired by
system, digestive system, and locomotor system. On the other the structure and the micro-suckers of an octopus, they deliv-
hand, non-invasive applications are associated with biophysical, ered an inexpensive and ultra-sensitive skin adhesive graphene-
environmental, and chemical stimulation, and they are mostly coated fabric (GCF) sensor that is sensitive to pressure and strain.
hard to monitor. Through this sensor, it can monitor a wide range of activities
of the human body efficiently, including wrist pulse, movement,
heart rate, and many other physiological signals. Moreover, it can
4.2. Electronic Skin and Multifunctional Sensing also detect speech vibration and wrist bending, even in wet sur-
roundings. This skin-adherent sensor has huge potential in the
Natural skin is a combination of various senses and activities, future (Figure 11a). Ye et al.[33] fabricated a sensor that has spe-
such as flexibility, intelligence, high sensitivity, quick response, cific sensing with directive selectivity with a femtosecond laser
and a built-in healing process. The urge to create a skin-like sen- fabrication process (Figure 11b). They could determine different
sor that can function as an intelligent sensor with multifunc- kinds of faults and defects in graphene in the laser patterning
tional capabilities drove the researchers to draw inspiration from system. Some specific patterns (i.e., basically four fundamental
natural skin. Furthermore, because of its self-healing properties, patterns: square, arrays, triangle, circle, and hexagon with right,
the skin part can easily recover the mechanically injured part on none, obtuse, and acute angles) of imperfect graphene were in-
its own.[162] The PC/rGO/PVA hydrogel with PC/rGO composite troduced, and they could be controlled and minimized by the
and PVA-borax hydrogel has been a bionic tactile component, fab- laser patterning process. They evaluated the sensing capability
ricated by Liu et al., and this solution propagates the way to pre- of graphene with different patterns, and correspondingly, a cir-
pare the electronic skin from PC/rGO/PVA hydrogel, necessarily cle pattern was used for strain fluctuation, a triangle shape for
assembled electrodes and adhesives. PVA-borax can activate self- temperature monitoring, and a hexagon for having information
healing effects, and it also improves biocompatibility and com- related to gas sensing. This sensor can essentially be integrated
pensates for the poor elasticity. The mutuality of PC/rGO and with e-skin and can perform various necessary sensing activ-
PVA-borax in the hybrid hydrogel makes it more amenable to ities like temperature detection, pulse, heart rate, and detect-
having the sense of skin epidermis, i.e., it can sense squeezing ing detrimental gases adjacent to the human body or clothing.
and stretching, mood conditions (emotional, happiness), recog- Gelatin nanofiber films have a much higher failure tensile stress
nizing the voice, and likewise.[162c,163] (35 MPa) and mostly possess better mechanical properties than
With the idea of the human fingertip, a micro-structured fer- many plastics like polyethylene and polysulfones. As a result, Liu
roelectric skin has been fabricated by Park et al.[164] with the et al.[167] fabricated GO film-based sensors to incorporate as e-
composition of rGO and PVDF composite film, and they com- skin for cardiovascular monitoring, and they used highly tough
prise a layer to retrieve the sensing information with the piezo- and robust gelatin nanofiber to ensure its durability (Figure 11c).
electric and piezoresistive properties accordingly. The micro- The sensor can perform activities like apexcardiogram record-
structured skins, which can easily separate them according to ing, sound recognition, and pulse spectrum evaluation and mon-
different surfaces, could have captured dynamic or static tactile itoring. Apexcardiogram recording is quite an essential element
stimuli like pressure, temperature, and acoustic waves. How- for hemodynamic and cardiac health recognition. It can monitor
ever, the E-skin has gained great interest for the nature of ventricular contraction, diastole, systole, blood ejection, atrioven-
the sensor as well as its spatiotemporal sensing and trans- tricular valve direction, semilunar valve open/close, and general
duction abilities.[164] Octadecane-implemented titanium dioxide valve open/close. With the input unit connected as an e-skin, the
nano capsule (OTNs)-graphene/PU film has been utilized with device can be used for cardiac health monitoring even with just
flexible wearable electronics by Chen et al.[165] this material pro- a mobile phone.
vides properties like thermal insulation, self-healing, and ultra- Human skin’s tactile sensing is quite complicated to imitate,
violet protective properties. The ductility and sensing properties and thus, fabricating a flexible and multifunctional E-skin with
have been amazing both before and after healing because PU higher tactile sensitivity has been a tough task in terms of mim-
has the self-healing property as well as the H-bonds and disul- icking the sensing attributes of human skin. However, sensitivity
fide bonds. The peak remained intact even after being cooled has been a crucial factor for the smart sensing E-skin as it has to
down and heated 20 times, which set up the notion that the de- maintain the properties to sense vibration, ambiance, environ-
vice had great thermal insulation. Most surprisingly, the coated ment, temperature, and different shapes and materials.[164,168]
fabric showed great resistance to UV radiation due to the pres- Proper flexibility, sensitivity, and quick responses to commands
ence of TiO2 , which is quite amenable to absorbing UV light. The in a sensor can even make it act like a humanoid robot. Moreover,
soft robots coated with the electronic skin on the prosthetic fin- these robots can modify objects and get the essence of the living
ger can perform a lot of activities through these important skin beings around them. Researchers assumed that someday this
attributes. This invention aligns with artificial intelligence, and robot would mimic human nature and function even better than
when it combines with the composition of hydrogel and PC/rGO, the somatosensory system present in the human body. Among
properties like strain sensitivity (higher sensitivity up to GF = all the efforts made on developing a multifunctional E-skin
14.14), stretchability (>5000%), compliance (≈1 mm), and self- with specific sensors, a self-powered E-skin with triboelectric

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Figure 11. E-skin in different healthcare monitoring applications a) graphene-based skin-adhesive fabric sensor for e-skin. Adapted with permission.[166]
Copyright 2019, American Chemical Society; b) graphene-based wearable sensors with pattern directive sensing fabricated by femtosecond laser fabri-
cation. Adapted with permission.[33] Copyright 2023, John Wiley & Sons c) GO films form gelatin nanofibers as e-skin for cardiovascular monitoring,
Adapted with permission.[167] Copyright 2023, John Wiley & Sons.

nanogenerators’ integration has been developed by Wang compared to mechanical signaling devices.[171] Electrophysiolog-
et al.[168a] and it could perform simultaneous pressure sensing ical signals are necessary for the treatment and prevention of pa-
and monitoring, temperature sensing, and recognizing the tients.
materials.[169] Wearable sensors have come a long way with the crucial
development of multi-sensing applications regarding real-time
monitoring of biosignals and many other non-invasive signals.
4.3. Electrophysiological Signal Monitoring However, many researchers raised the issue of the comfort of
the wearables, as the device has to be carried along with the
Graphene-based wearable sensor is basically another feather in wearer. Ali et al.[172] fabricated wearable fabric-based electrodes
the cap of medical science in the modern era of smart transduc- with graphene materials that can exhibit enhanced, real-time,
ers, electronic materials, and smart wireless systems. That is why and stable biosignal detection ability. This study revealed a com-
it has attracted such interest in the community of researchers. fortable and flexible method to fabricate electrodes to monitor
Electrical activities have a lot to say about health conditions be- and evaluate ECG signal detection, and they just developed the
cause the human body is more likely to be made up of chemical sensor by depositing a graphene-based nanocomposite over the
and electronic systems via mechanical structures.[58b,161,170] As a fabric substrate. By getting out of the very traditional methods of
response to the demand for low-cost, reliable, and easy disease fabricating electrodes, they reduced the importance of gel in the
detection and monitoring, miniature instruments in medical fabrication of sensors. Moreover, it can stay directly in contact
science such as portable electrocardiography, glucometers, elec- with the skin. Most of the results of the study come from values
tronic sphygmomanometers, and paper-based diagnostics have of a higher signal-to-noise ratio (SNR) with lower skin-electrode
already been invented. Thus, these instruments can alleviate the impedance. Hence, the ECG signals could maintain a supe-
hospital’s burden by detecting chronic disease early and precisely, rior quality and effectively distinguish all crucial ECG signals
as well as keeping a record of the long-term physiological condi- according to their important features. For example, 40 dB was
tion to ensure continuous health monitoring. Long-term electro- the range of the ECG signal-to-noise ratio (SNR) according to
physiological signal monitoring via wearable sensors with physi- the record in the monitoring devices. In addition, it is worth
cal and cognitive functions has become popular for health mon- noting that the ECG signal intervals during each cardiac cycle
itoring and diagnosis. Therefore, these devices are more stable exhibit little temporal fluctuation. The electrodes can be utilized

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multiple times following washing due to the presence of the excellent fast response time and relaxation time of 0.5 s, which
superhydrophobic characteristic. In conclusion, the PVDF/GNP made the device more flexible in bending-stretching response.
electrodes that have been produced exhibit several desirable Most importantly, the sensor can easily generate and moni-
characteristics, including reusability, biocompatibility, effective tor electroencephalography (EEG), electrocardiography (ECG),
skin-electrode interaction, and the absence of skin irritation. and electromyography (EMG), showing better biocompatibility
This research holds promise for more comfortable and effective than was tested with a cytotoxicity test. Zhang et al.[177] fab-
ECG signal detection, with potential applications in healthcare ricated a portable, flexible, and multimodal on-skin graphene-
and biomedical monitoring. The non-intrusive nature of wear- based sensor for electrophysiological signal monitoring with low
able electronic textiles (e-textiles) made of graphene bodes well impedance (Figure 12b). The on-skin electrode sensors in a wire-
for the next generation of personalized healthcare applications. less communication module can essentially exhibit the three-in-
However, their broad use is restrained by inferior performance, one attributes of monitoring ECG, EMG, and EEG. Additionally,
decreased comfort, and increased material costs. Wearable it makes the device more comprehensive for medical applications
e-textile sensors based on graphene have been developed by and the field of wearable sensors. This low-cost ($25) and very
Tan et al.[173] for bio-signal detection; they are highly scalable, light-weight (22 g) solution can provide real-time electrophysio-
sensitive, and ultra-flexible. An optimized two-layer sensor was logical signal monitoring, and the human-machine interface with
further assessed as a breathing sensor to gauge the practical a mobile app can provide the services of fitness tracking, diag-
bio-signal sensing potential of the piezoresistive sensors. In nosis, and very easy health check-ups from time to time. Qiu
the supplementary material, the plux system was employed as et al.[178] fabricated graphene-based wearable sensors inspired
a reference measurement, positioning the dual-layer sensors by the structure of the avian nest (Figure 12c). They produced a
beneath the plux elastic band at the chest’s center. The sensor skin electrode to detect electrophysiological signals from a semi-
was also incorporated for recording resistance shifts during embedded and highly graphitized electro-spun fiber/monolayer
breath analysis. These two-layer piezoresistive sensors exhibit graphene (GFG)-converting soft elastomer for making the con-
the capacity to function as wearable sensors for both human ductive film. The sensor showed a higher conductivity of 150 Ω
movement and bio-signal detection, characterized by their rapid m−1 and stable electrical performance with biometric signals.
response and recovery times. A novel and facile technique has Therefore, as an alternative, the dry electrodes are more com-
been described in this study for making electro-conductive yarn patible and easy-going for the patients. as they can maintain good
out of graphene, which could then be embroidered into piezore- contact with the human body during movement and even dur-
sistive sensors. The multilayer sensors were more sensitive, ing exercise. After a lot of attempts, various dry sensors have
responded quickly, and recovered from failure quickly. been fabricated, like conductive elastomers, conductive fabrics,
There are a lot of electrical phenomena that have been pro- and metal-type electrodes. Their rigid structures and the greater
duced from the human body as well as the animal tissues prior contact impedances create discomfort for the wearers, and some-
to the active cells, and they are mostly known as the “bioelec- times they may cause damage to the skin after a long time. There-
trical signal.” Due to the transmembrane flow of the ions, the fore, in search of flexible materials, the researchers found dry
resting potential (RP) and the action potential (AP) follow the sensors made from CNTs, PDMS, and rGO that were easy to
mechanism of bioelectrical signals. The potential difference be- implement. As most of these are quite expensive to fabricate,
tween the inside and outside of the cell membrane produces the they found thermally reduced graphene oxide to be one of the
static potential, whereas the active potential comes from the cell’s best candidates for a biocompatible and cheap sensor material.
stimulation when it is excited from the outside. As the initial However, there was some concern about TRGO toxicity when it
membrane potential rises, there are a series of transient changes came into contact with the human body.[175a,179] Surprisingly, Das
followed by a certain recovery but a slow approach to the rest- et al.[176] developed an excellent high-performance and paper-
ing potential.[174] Additionally, electrodes are mainly the sensing based epidermal sensor that is placed over the biocompatible ny-
component in the device for capturing the signal from the human lon membrane (NM), and the most important thing is that they
body. With the help of silver/silver chloride (Ag/AgCl) electrodes, did not use any detrimental elements in the process. The epider-
the wet electrodes were fixed on the human body to evaluate the mal sensors under the conventional tattoo have been fabricated
bioelectricity from several physical activities, in the conventional with metal films and silicon membranes by Ameri et al.,[62c] and
methods. As the wet electrodes possess a high risk of skin irrita- they came up with a method called “wet transfer, dry patterning,”
tion and allergic reactions to the gel and adhesive materials, the which was cost- and time-effective and known as graphene elec-
wet electrodes are not that amenable in the long-term. Moreover, tronic tattoo (GET). The sensor, with a thickness of 463 ± 30 nm,
it has been reported the irritation may last even longer than 12 higher sensitivity (>40%), and excellent adhesion to the skin,
hours in the body of the patient and it requires a replacement of could capture various bioelectrical signals, including the ECG,
the gels once they get dry.[175] EEG, and EMG. Moving forward, low-cost, high-performance
Das et al.[176] fabricated a wearable sensor to monitor hu- bioelectrodes have been developed by Yun et al.[180] through the
man motion and electrophysiological signals (Figure 12a). They solution-based method with rGO and porous polydimethylsilox-
adopted a vacuum filtration process with GO and nylon mem- ane (PDMS). Moreover, they were highly stretchable (strain>
branes, and they used no harmful elements or chemicals in the 149%), durable (up to 5000 cycles), and low sheet-resistant (1500
entire process. The docile process can fabricate an epidermal sen- Ω−2 ) which denoted their potential for the world of wearable sen-
sor with high sensitivity and a sheet resistance of 40 Ω sq−1 . as sors at a very low cost. A multifunctional on-skin electrode with
the impedance in skin contact was ≈20 kΩ at a very low fre- laser-patterned porous graphene had been fabricated by Sun et al.
quency. With an amenable tensile strain, the sensor showed an and could exhibit a superior water-vapor permeability of 18 mg

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Figure 12. Graphene-based wearable sensors for electrophysiological signal monitoring. (a) Thermally reduced graphene oxide and nylon membrane-
based sensor fabricated by vacuum filtration for monitoring electrophysiological signals. Adapted with permission.[176] Copyright 2023, Elsevier Limited.
(b) Portable wearable sensors with low-impedance graphene electrode sensors for electrophysiological monitoring. Adapted with permission.[177] Copy-
right 2022, Wiley VCH-GmbH. (c) A transparent and bioinspired graphene electrode sensor for monitoring electrophysiological signals. Adapted with
permission.[178] Copyright 2020, American Chemical Society.

cm−2 .h−1 and a water-wicking rate of 1 cm/30 s. Because this sen- vented. As the IR devices and thermal imaging cameras were
sor can also monitor air permeability and reduce the risk of in- able to provide the temperature without any contact with the
flammation, it can also address the issue of comfort and is better surface, this idea helped to come up with the idea of devel-
for long-term monitoring.[181] As a result, all biophysical and elec- oping wearable temperature sensors with the ability to moni-
tromagnetic signals can be captured by graphene-based wearable tor the temperature in dynamic environments and places with
sensors, including EEG, ECG, EOG, and EMG, while maintain- spatial variations.[23] Although thermocouples,[182,183] thermos-
ing their strategy and principles.[174a] resistance,[184] and thermal-responding field-effect transistor-
based temperature sensors[185] have come a long way, they fail
to provide a wide range of thermal properties. However, deli-
4.4. Therapeutics and Temperature Sensing cate electronic circuits are necessary so that the device can pro-
vide accurate detection. To form efficient, flexible thermal sen-
Temperature has been a crucial parameter for the physiolog- sors, graphene is one of the most superior elements because of
ical monitoring of the human body and monitoring health- its exceptional electrical, physical, thermal, and chemical prop-
related problems, as having precision and accuracy in body tem- erties. The exceptional thermal properties make graphene differ-
perature is quite important to monitor continuously. Although ent from any other material in terms of fabricating a temperature
there was an abundance of material with the ability to pro- sensor. Moreover, it has an excellent thermal-responsive ability to
vide good resolution and accurate temperature measurement, provide a great temperature-sensing application.[186]
they are mostly contact-based and rigidly shaped, which makes For optical transparency, conductivity, carrier mobility, and
them not so suitable for the body’s long-term usage. There- flexibility, graphene materials are selected for different micro-
fore, real-time temperature monitoring became a great chal- electronics and sensors. In terms of biosensing, active electro-
lenge to execute.[23,182] Localized temperature sensing has been chemical defects due to low-density graphene deposition have
quite problematic because the body surface is not flat. Therefore, been a limitation in the development of graphene-based sensors
measuring and monitoring the temperature from the curved for thermal and therapeutic applications. Lee et al.[52] fabricated
surface as well as defining the signals from the skin’s sur- the wearable sensor with gold-doped graphene in a gold mesh
face considering the consumer’s mobility have yet to be in- with electrochemical activity that can create a patch so that it can

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Figure 13. Graphene-based wearable sensors in thermal and therapeutic applications a) reduced graphene oxide-based strain sensor for monitoring
temperature sensing in healthcare. Adapted with permission.[187] Copyright 2023, Elsevier Limited. b) Incorporation of graphene flakes to produce
graphene-based wearable sensors for thermal sensing. Adapted under the term of Creative Commons Attribution License 4.0 (CC BY).[189] Copyright
2019, The Authors, published by American Chemical Society.

evaluate and remark on the diabetes condition of the patients. mal pad with a communication module can monitor tempera-
Moreover, it can also generate precise feedback for the wearer. ture continuously, and it has been proven by different trials on
A heater with different sensors (i.e., temperature, pH, humidity, animals. Most smart wearables are generally integrated with sen-
and glucose) and a polymeric and thermally activated micronee- sors in the body, textiles, or materials. However, manufacturing
dle for drug delivery are the main components of this wearable smart textiles by using conductive yarn was quite expensive be-
sensor. This sensor can smoothly deliver metformin to reduce fore Afroj et al.[189] introduced the docile, ultrafast, washable, and
the diabetes level in the bodies of diabetic mice. Nanofiber com- highly scalable graphene-based textile sensor, where graphene
posites with conductive polymers for wearable sensing devices flakes were dispersed to coat the textile yarn with graphene ink
are now quite popular due to their flexibility and high precision (Figure 13b). In its knitted structure, the graphene-based wear-
in different biomedical attributes. However, this innovation still able can essentially send information regarding health continu-
faced some challenges in maintaining proper wetting properties, ously. Most importantly, it can sometimes work in self-powered
durability, and multifunctional sensing operations. Xiao et al.[187] mode for a low-powered Bluetooth in an RFID system. It showed
fabricated a multifunctional graphene-based strain sensor with superior thermal sensitivity and conductivity. It projected a high-
rGO and a polymer nanofiber core that can essentially be used scale production rate of 1000 kg/h for fabricating electroconduc-
as a temperature sensor for high-performance functional uses tive yarns.
and biomedical applications (Figure 13a). Moreover, it can also be For flexible temperature sensors to be useful in real-time
used for body motion monitoring, and it showed high sensitivity wearable health care, they must have high sensitivity, great lin-
with great durability for >1000 cycles of use. Thermal imaging is earity, and wireless monitoring. Particularly demanding sensor
an essential part of human condition evaluation, and it helps to performance is the multichannel body temperature monitoring
provide a general idea regarding the human body and hints for system, which must constantly keep tabs on a massive volume of
different diseases. Moreover, heat therapy and thermography are data. Chen et al.[190] designed a system for wirelessly monitoring
used to cure many diseases and injuries in the skin tissue. Kang body temperature that makes use of an in-situ temperature sen-
et al.[188] developed a graphene-based patch for thermal monitor- sor array with high sensitivity and excellent linearity. The porous
ing used in thermal distribution and evaluating thermography. graphene/polydimethylsiloxane sensing layer allowed them to
The thermal patch can keep track of continuous skin tempera- create a flexible temperature sensor. In the region of 30–70 °C,
tures for sensing and generate thermography for self-care treat- this sensor showed both high sensitivity (5.203% °C−1 ) and excel-
ment facilities. The capacitive sensor in the graphene-based ther- lent linearity (R2 = 0.996). These high-performance temperature

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sensors have found use in a variety of contexts, including the strates the applications of graphene-based wearable sensors. The
monitoring of human body temperature and breath in both nor- sensors can also help in combating pandemics, and some of the
mal and abnormal breathing rates. To further facilitate distant brilliant research regarding pandemics and the ways to fight fu-
and multichannel body temperature monitoring, the researchers ture pandemics has been demonstrated in the following section
set up a high-throughput wireless body temperature monitoring of this review.
system consisting of wireless sensor modules, a cloud server,
and a portable electronic device. Thermal imaging is an effective 5. Graphene Sensors in Tackling Future Pandemics
method for evaluating a patient’s health and aiding in the diag-
nosis of a wide range of medical disorders. Heat therapy, often The side effects of COVID-19 have still been around in the post-
known as thermotherapy, is also effective in treating damage pandemic environment. Due to its different routes of transmis-
to the skin and other superficial tissues. In this research, we sion, the extremely contagious spread of the viral infection was
introduce a thermal patch that may be worn to simultaneously almost impossible to stop. Therefore, it is important to become
give thermotherapy and track the user’s skin temperature in real- more aware of and prepared for pandemics. Graphene-based
time. This cutting-edge tool provides a highly efficient self-care wearable sensors can play a vital role in defending against the
option. For the purposes of thermography and temperature dis- foreshadowed pandemics in the future, as we never know when
tribution mapping, Kang et al.[191] developed a wireless graphene- they may happen. Furthermore, due to overuse and overexploita-
based thermal patch. The system consisted of a capacitive sensor tion of resources, the implementation of sustainable products
based on graphene, a thermal pad made of graphene, and a flexi- with properties such as ease of fabrication, resource and cost ef-
ble readout board that was paired with a wireless communication ficiency, environmental friendliness, and lower energy require-
module. The wearable sensor exhibited continuous monitoring ments is now unavoidable.[225] The laser-induced graphene mate-
of temperature fluctuations across a significant surface area of rials from the single-step laser scribing can fight against the coro-
the skin, measuring 3 × 3 cm2 , with remarkable precision and naviruses HCoV-OC43 and HCoV-229E and destroy the virus
sensitivity. In addition, thermotherapy was implemented by in- within 15 minutes of photothermal action. By adding metal and
corporating a heater based on graphene, which was positioned at metal oxides, the nanofibrous textured edges could enhance their
the bottom of the device. The diagnostic capability of the system antibacterial effects. The highly conductive property improved its
for many diseases has been verified through animal tests. joule heating properties as well as its self-sterilization into air and
A flexible temperature sensor has been fabricated by Rogers water. The oxygen overpotential enabled the great electrochem-
et al. and implemented over the serpentine gold and PIN diodes ical properties. Aside from that, the LIG can destroy microbes
with Si nanoribbons on elastomers.[192] The flexible Ni-polymer using hydrogen peroxide, putting the microbes under oxidative
composite-based sensor worked with a wireless connection that stress. Electroconductive filters made of LIG can be used in high
covered a very short dynamic range (25 to 400°C) and it was in- flux and have been coated with PVA and GO. The membranes can
troduced by Bao’s team.[184a] With the help of a bimodal sensor kill microorganisms with their very high flow rate and in flow-
array, Park et al.[193] came up with the idea of continuous and through mode. A lot of researchers are interested in using LIG
simultaneous sensing of pressure and temperature, and those in wearable sensors because it has the best texture, conductivity,
sensors can monitor the precise and regular thermal state of the and durability of the membrane surface. Additionally, LIG’s re-
human skin. Unfortunately, they provided an inferior thermal re- markable self-sterilization properties and the fabrication process
sponse. As a thermally sensitive element in conventional micro- have been recognized for their immense potential as a control
nanofabrication techniques, monolayer or bilayer graphene was and prevention technology.[226]
deployed on silicon materials. However, it fell behind as there When graphene was incorporated into conventional LFP
was a lack of flexibility. As a solution to it, Trung et al.[186b,c] (lithium iron phosphate) batteries, they were charged way faster
suggested a flexible temperature sensor with the ability to de- than lithium-ion batteries. Furthermore, those have the advan-
tect slight changes in temperature. That experiment was imple- tages of being lighter and having a larger capacity. Figure 14 il-
mented by polymer substrates with the reduced graphene oxide lustrates the use of graphene in detecting COVID-19 and prevent-
thermal-responsive field impacting the transistor. Then again, ing its spread through protective measures. Therefore, it can be
the stretchability and the temperature responsibility were quite advantageous to the sensors operating with graphene-based ma-
inferior and limited. Finally, the graphene nanowalls (GNWs) terials too. A graphene-based sensor with the ability to capture
from the graphene nanosheets vertically over the substrate pro- the real-time detection of tiny molecules has been fabricated by
vided a floor for the gas sensor and the biosensors. That used to Cardea (presented by San Diego Nanomedical Diagnostics).[227]
have great stretchability to a greater extent for the vertically stand- A resistive biosensor made of graphene has been deployed to
ing graphene nano walls that are perpetually interlaced. There- detect the COVID-19 virus with a graphene-modified electrode.
fore, it enabled the material to be flexible, stable, highly sensitive, The hepatitis B virus was detected with a composite of reduced
and a simple temperature-responsive material.[194] There are still graphene oxide and gold nanoparticles, and it happened within
several fields in graphene-based temperature sensors requiring a very short detection limit. A rGO nanocomposite with gold
more research and their performance and efficacy have not been nanoparticles was used to detect diarrhea. Single-layer graphene
up to the mark yet. is also applicable in biosensing applications for its robust ther-
All these applications are quite eminent in healthcare in the mal conductivity, good elasticity, high mechanical strength, and
modern world. Since healthcare is too expensive and inaccessible greater surface area.[228] Graphene was driven to detect the SARS-
in so many countries, these technologies can bring solutions at a CoV-2 virus in the laboratory of the University of Illinois at
very cheap price to the people of those countries. Table 3 demon- Chicago by their researchers.[229] The single-atom-thick carbon

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Table 3. Applications of graphene-based wearable sensors.

Applications Sensor-type Materials Attributes

Reference

Human movement, Pressure Carbon black/silicon elastomer composite Outstanding compressibility with better air [195]
gesture, and health on warp-knitted polyester fabric permeability and greater moisture
monitoring management.
Pressure PEDOT on PVDF nanofiber Wearable computers and healthcare devices [196]
Pressure rGO on Nylon fabric Detecting both force and position precisely [197]
Measurement range: 2500 kPa
Sensitivity: 5.2 ΩkPa−1
Strain Nano-plated epoxy graphene on glass fiber Very high gauge sensitivity [198]
Strain Ecoflex graphite on silk fabric Human-motion converted music production for [199]
different instruments.
Strain rGO/PDMS on PU and PE fibers Detecting multiple kinds of deformation in fiber [200]
Strain Ecoflex on nylon The gait of the patients can be monitored with [201]
better rehabilitation assistance and
augmented human work-rate evaluation with
respect to muscle work
Strain Silicon rubber and multi-wall carbon Gesture recognition and motion monitoring [202]
nanotube with rotational angles and axial joints
Strain ZnO nanowires with polyurethane fibers Highly stretchable (up to 150%) and can detect [203]
strain, temperature, and UV level
Strain Stencil printing silver ink Detecting and converting full-range finger’ [204]
movement with a wireless control system
Strain VGr nanowalls Greater stretchability and detecting of sound [205]
amplitudes
Strain Polyurethane and brittle conductive Heartbeat monitoring, pulse rate, sound signal [206]
nanowires/graphene particles acquisition, and recognition
Triboelectric Elastic rubber and aluminum film Breathing and joint motion capturing. [207]
nanogenerator
(TENG) based
Electronic skin and Strain rGO with PDMS Analyzing human electrophysiological signals [208]
Multifunctional Tactile sensor Carbon nanofiber Higher conductivity [209]
sensing
AgNWs with GO Real-time monitoring of electrocardiogram [210]
(ECG) and electroencephalogram (EEG)
signals
P(VDF-TrFe) with rGO Mapping of spatial pressure distribution with [211]
monitoring the human physiological signals.
Strain Substrate-free laser-scribed graphene (SFG) ECG detecting system based on GES [212]
with silicon
Strain PDMS with rGO Human motion monitoring [213]
Strain In2 O3 and Se with graphene Robotics and human-body motion monitoring [214]
Electrophysiological paper-based Chemically modified graphene (CG) and Comfortability and a high sensitivity for [215]
signal monitoring physiological carboxylic multi-walled carbon nanotube electrocardiogram signal detection
sensor composites
AI-based on-skin Multimodal Data acquisition (DAQ) unit Tracking fitness updates and essential medical [216]
sensor with soft materials diagnostics with a human-machine interface
Biosensor Dry electrode design on graphene ECG monitoring [217]
(GN)-based electrochemical
nanomaterials
On-skin sensor rGO Healthcare and health machine interface (HMI) [218]
Strain Molybdenum diselenide (MoSe2 ) Pulse rate monitoring, skin hydration sensors, [219]
interspersed with polyvinyl alcohol (PVA) and human gesture recognition
AESR-based 3D-PAS with multiple electrodes and AESR Sensing interfaces with curved auricular skin [220]
Hydrogel Graphene oxide (GO) with polyvinyl alcohol Continuous capturing of human body motion [221]
(PVA) mixed with polydopamine (PDA) and recognizing physiological parameters
(Continued)

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Table 3. (Continued)

Applications Sensor-type Materials Attributes

Reference

Temperature sensing Metal-based rGO Superior sensitivity to temperature, good [189]

electroconductive washability, and excellent flexibility
strain Femtosecond Laser Fabrication Measuring body pulse, gas inside the body, and [222]
temperature with clothes, as well as real-time
health check-ups and protection signaling
Freestanding rGO Healthcare and biomedical monitoring [223]
fiber-based
Pressure rGO on polypropylene nonwoven fabric Human body movement and motion [224]
Strain Conductive polymer nanofiber composites Capturing body motion with the negative [187]
(CPNCs) temperature coefficient effect (NTCE)

material could make resonant vibrations. Furthermore, the vi- bat pandemics in the future. According to the WHO, frontline
brations could be precisely counted, which became known as workers are suggested to wear graphene-based facemasks that
phonons. The resonant vibration plays a very specific role as it might minimize the transmission of the virus. The research fo-
dismantles the structures of SARS-CoV-2 molecules as soon as it cusing on wearables, sensors, and functional textiles must be
interacts with graphene. The research to develop graphene-based stepped forward so that the technology can be useful in terms of
sensors at the atomic level to detect COVID and cancer.[230] controlling and protecting from the spread of viruses. Graphene-
Graphene has a strong antibacterial impact due to its high based wearable sensors play a vital role in the pandemic. More-
inhibitory capability. The composite antivirals are made up of over, graphene facemasks are recyclable by the photocatalysis
sulfate, heparin, and graphene. The antiviral activity against the method or the thermal setting process. The titanium oxide and
African virus was discovered in rGO sulfate compounds cre- silver nitrate coating over the graphene materials can deteriorate
ated for thermal power. DPG (dendritic polyglycerol) with sul- the virus at a mild temperature within ≈ 30 min.[34b,233] Moreover,
fation, incorporated with rGO could detect various orthopoxvi- the sensors are always there to detect and provide the necessary
ral strains by working as an antivirus. A carbon blanket restricts information. Research must go on about this topic, and the study
the micro-organisms from growing, and the GO flakes are used on graphene-based wearable sensors will surely bring out some
to do the main job at that place. SARS-CoV-2′s protein recep- outstanding technology for any future outbreaks or pandemics.
tor agent is used to interact with heparin and modify its own
conformation.[230,232] 6. Perspectives, Challenges, and Conclusion
Graphene has been known as an outstanding antiviral sub-
strate to fight against the spread of viruses, diseases, and infec- Graphene is now being used as a sensor and signal transducer
tions. As a result, graphene-based wearables may be able to com- in various wearable and mobile health device prototypes. More

Figure 14. Application of graphene-based wearable sensors in tackling COVID-19 and future pandemics.[231]

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interestingly, graphene has paved the way for the use of other 2D structure and the mechanism of action of graphene is necessary
materials in sensors and mobile health-monitoring devices. The to derive efficient properties from it. Therefore, more research on
various types of sensors discussed here revealed that for high- controlling the factors with minimal environmental impact can
performance sensors, the right combination of doping materi- build a sustainable future by ensuring large-scale production of
als, device architectures, and synergistically contributing interfa- them.
cial effects is critical. Recent research promotes the utilization of In the case of manufacturing graphene wearable sensors, there
graphene and its derivatives, along with the functionalization of are two primary units: 1) conductive mesh, which functions as a
graphene with other substances, as a sensing material in a wide signal-capturing device; and 2) flexible substrate, which provides
array of wearable sensors. Due to the multifunctional properties protection to the conductive mesh and also functions as a base.
of graphene-based materials, this review paper focuses on newly Therefore, the substrate materials need to be chosen carefully to
developed graphene-based wearable sensors for detecting tem- impart optimum flexibility and protection. Though the graphene
perature, gas, strain, piezoresistive pressure, various chemical electrodes are flexible, stress corrosion cracking has been no-
detections, and electrophysiological signals. In addition, this re- ticed, especially during ECG, due to enhanced electronic impu-
view shows that graphene can detect a wide range of signals. This dence that resulted in low sensitivity.[237] Some novel techniques
allows researchers to explore how graphene can be used in wear- are currently being studied to enhance flexibility and durability.
able health monitoring devices that work in real-time. These de- For instance, bridging materials like silver nanowires or carbon
vices are getting a lot of attention from researchers across many tubes can be incorporated to improve mechanical stability. Again,
fields because they can track important body functions and find lubricant can be used to reduce the stress on the strain sensors.
diseases early. Graphene-based wearable sensors show promis- Also, a brick-and-mortar structure can be developed between the
ing advances as an emerging technology that will have a positive substrate and nanomaterials by forming ionic bonds and 𝜋−𝜋
impact on healthcare. Nevertheless, it is still suffering from mul- bonds that will increase the overall stability of the sensor.[238] Af-
tiple challenges and limitations that need to be addressed. ter all, to overcome this issue, the selection of processing method,
The first and foremost drawback of graphene application is substrate, and compatibility should be considered carefully. Fur-
the difficult and complex synthesis process. Different types of ther study is needed to detect the reasons for the poor sensitiv-
production processes have already been developed, but unfortu- ity and durability of the graphene wearable healthcare sensors.
nately, all of them have some individual benefits and shortcom- It is also noticeable that graphene-based wearable sensors show
ings. For instance, the chemical vapor deposition process is one a narrow sensing range to detect signals, which can be inap-
of the most promising methods to synthesize graphene on an propriate for real-world applications. Thus, highly sensitive sen-
industrial scale due to its large and top-quality graphene pro- sors with a wide range need to be developed through further
duction with controllable layers, but the transfer process of this study. Furthermore, comfort is a mandatory property for wear-
method is not efficient. Again, the exfoliation method is cheap able sensors. It has been found that wearable sensors use con-
and simple, but the size and layers of graphene cannot be con- ventional tape or bandages to attach the sensors to the body
trolled properly. The researchers are still facing challenges in pro- or skin, which could be annoying for the users. Hence, self-
ducing high-quality graphene on a mass scale at a cheap cost. In adhesive wearable sensors need to be developed, which is possi-
the current scenario, the processing cost of graphene is much ble by using gecko-inspired microfibers, ultrathin packaging, mi-
higher compared to similar carbon materials like activated car- croneedle arrays with swellable tips, or chemical adhesives (e.g.,
bon, which limits its application on a broad scale. To overcome polydopamine)[239] In addition, sweating is a usual bodily func-
this issue, more research is required to develop and upgrade the tion that needs to be vaporized properly. Wearable clothes should
synthesis methods for graphene.[234] Besides, another matter of not be an obstacle to sweat vaporization from the skin. Thus, the
concern is the biocompatibility of graphene-based composites. wearables must be breathable, which can be obtained by using
It has been found that some of them are biocompatible, and textiles or a 3D sponge to fabricate the sensors, which will also
again, some are toxic.[235] The toxicity of graphene has been ex- increase their flexibility. Besides, graphene-based wearable sen-
plored in fish, plants, fungi, bacteria, and animals. The impact sors need to show responses only based on the human body with-
of graphene on these organisms is mostly negative and varies out considering environmental factors. However, as graphene is
from one to another. The possible ways of graphene leaching a very sensible material, it may show different responses due to
are graphene production, graphene-based wearable manufactur- changes in temperature, moisture, or pH values.[238] As a result,
ing, graphene-based wearable use, reuse, and recycling, and un- graphene-based wearable sensors need further study to protect
planned disposal of graphene-based wearables.[236] To decrease their responses from outside factors. Hydrophobic coatings and
the exposure of graphene to life, the production of graphene thermal insulator material can be utilized to make them water-
needs to be secured, standards need to be followed for the care proof and thermally stable. For the long-term use of wearable sen-
and laundry of graphene-based wearables, and the disposal of sors, sustainable power sources can be an issue that can be mit-
graphene-based wearables has to be done more safely. The hu- igated by incorporating a self-powered generator. For instance,
man health and environmental impact of graphene also need to a triboelectric nanogenerator can harvest energy from the envi-
be considered for further study to make it more sustainable and ronment and human movement[240] which can be incorporated
human-friendly, especially the exfoliation-based synthesis tech- with graphene-based wearable sensors for self-powered capabil-
niques. Reproducibility and recycling of graphene materials have ity. Future research can be focused on developing graphene-based
been an underlying demand in the current world. The success of wearable sensors that are lightweight, flexible, comfortable, sus-
biomedical devices depends significantly on their production and tainable, cheap, reusable, battery-free, and multifunctional with
processing methods. Also, an intensive study of the molecular a proper response to stimuli.

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Mahmuda Akter has been working as an associate professor at the Bangladesh University of Textiles.
She has completed her Ph.D. from Erciyes University, Turkiye, under the prestigious CoHE (Council
of Higher Education) Ph.D. Fellowship. Prior to that, Dr. Mahmuda obtained her B.Sc. and M.Sc. in
Textile Engineering from the Bangladesh University of Textiles (BUTEX). Before becoming a faculty
member of BUTEX, she had professional and industrial experience in textile factories. Her major fields
of study and research interests are wearable technology, graphene and 2D materials, textile materials,
fiber-reinforced polymer composites, textile structural composites, nanocomposites, biocomposites,
technical textiles, and sustainable materials.

Habibur Rahman Anik is an inquisitive graduate student, who is embarking on an exciting journey in
material science and polymer engineering. With a BS in Textile Engineering from Bangladesh Uni-
versity of Textiles, Anik has been devoted to the world of materials science. His research interests
span polymer chemistry, composites, fiber science, hydrogel, bio-based materials, and nanoparti-
cles, exploring intricate properties. Anik excels at identifying complex problems and crafting inge-
nious solutions. He aspires to become a formidable scholar in the field of smart materials, garnishing
his achievements with international acclaim through captivating presentations, groundbreaking re-
search, and inventive problem-solving.

Shariful Islam Tushar is currently pursuing his MSc from Oklahoma State University (OSU), majoring
in Apparel Design and Production. He is working as a Graduate Teaching Assistant at the Department
of Design and Merchandising of OSU. His research interest belongs to soft materials including fiber,
polymer, and textiles, and their inclusion with the Internet of Things (IoT). He graduated with a bach-
elor’s degree in Textile Engineering from the Bangladesh University of Textiles, Dhaka, Bangladesh in
2021.

Imana Shahrin Tania is an Associate Professor in the Department of Wet Process Engineering under
the Faculty of Textile Chemical Engineering. She is a fellow of the National Science and Technology
(‘NST’), Ministry of Science and Technology, Bangladesh. Dr. Tania has an outstanding academic
background. She completed her Ph.D. from the Bangladesh University of Engineering and Technology
(BUET). She completed her graduation and post-graduation in textile engineering with a specializa-
tion in wet process engineering from Bangladesh University of Textiles. Besides teaching, her prior
interest lies in effective research work. Her research interests focus on advanced functional finish-
ing, nanotechnology, surface modification, characterization of textile fibers, eco-friendly dyeing and
finishing technology, and technical textiles.

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Md. Kamrul Hassan Chowdhury is currently working as an assistant professor in the Department of
Apparel Engineering at the Bangladesh University of Textiles. He was appointed as a lecturer at this
university in 2017. He completed his B.Sc. in Textile Engineering with a specialization in Apparel En-
gineering from the same university; he also has an excellent industrial background, as before start-
ing his career as an academician, he worked in a leading knit composite factory in Bangladesh for >3
years. His area of interest for research includes advanced textile materials, textile nanocomposites,
advanced garment CAD systems, and supply chain management.

Shah Md. Maruf Hasan is serving as an assistant professor at the Department of Apparel Engineer-
ing under the Faculty of Fashion Design and Apparel Engineering at Bangladesh University of Textiles
(BUTEX). He was appointed as a Lecturer in 2019 at the same department at Bangladesh University
of Textiles. Prior to becoming a faculty member of BUTEX, he had professional and academic experi-
ence in private universities. His major field of study and research interests are wearable technology,
graphene, textile composite, additive manufacturing, life cycle analysis of products, etc.

Bebe Fatema Bristy is an undergraduate student in Textile Engineering from the esteemed Bangladesh
University of Textiles. Her academic pursuits were in the Department of Apparel Engineering, which
is housed under the Faculty of Textile Fashion Design and Apparel Engineering. Bristy’s passion for
research was sparked during her undergraduate studies in Textile Engineering. Since then, she has
excelled as a research assistant while maintaining exemplary academic performance. She has explored
various sectors of the textile field through her research projects, always striving to bring innovation to
the field. Her projects have included nanotechnology, smart textiles, LCA of denim apparel, superhy-
drophobic functionalized textiles, and apparel production systems. Looking to the future, Bristy has
ambitious plans to continue her academic journey while contributing to the textile industry in mean-
ingful ways with her unwavering commitment to research and impressive track record.

Adv. Sensor Res. 2024, 3, 2300120 2300120 (31 of 31) © 2023 The Authors. Advanced Sensor Research published by Wiley-VCH GmbH.