Advanced Materials - 2022 - Zarei - Advances in Biodegradable Electronic Skin Material Progress and Recent Applications in

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Advances in Biodegradable Electronic Skin: Material

Progress and Recent Applications in Sensing, Robotics,
and Human–Machine Interfaces
Mohammad Zarei, Giwon Lee, Seung Goo Lee,* and Kilwon Cho*
strain. The signals generated by these

The rapid growth of the electronics industry and proliferation of electronic stimuli are transferred to the central
materials and telecommunications technologies has led to the release of a neural network and brain to provide an
massive amount of untreated electronic waste (e-waste) into the environ- appropriate response. In addition, biolog-
ical skin possesses unique characteristics,
ment. Consequently, catastrophic environmental damage at the microbiome
such as stretchability, self-healing ability,
level and serious human health diseases threaten the natural fate of the and mechanical toughness.[1–3] It also pro-
planet. Currently, the demand for wearable electronics for applications in vides an effective barrier against ambient
personalized medicine, electronic skins (e-skins), and health monitoring is elements such as chemicals, gases, radia-
substantial and growing. Therefore, “green” characteristics such as biodeg- tion, and external biological agents.
radability, self-healing, and biocompatibility ensure the future application of Electronic skin (e-skin) is an artificial
smart skin composed of various electronic
wearable electronics and e-skins in biomedical engineering and bioanalytical
sensors distributed on a single uniform
sciences. Leveraging the biodegradability, sustainability, and biocompatibility surface or stacked on multiple surfaces.
of natural materials will dramatically influence the fabrication of environ- It mimics some of the biological skin
mentally friendly e-skins and wearable electronics. Here, the molecular senses and provides a promising sensing
and structural characteristics of biological skins and artificial e-skins are platform for key application areas such as
wearable sensors, robotics, and prosthetics
discussed. The focus then turns to the biodegradable materials, including
(Figure 1).[1,4–11] However, serious concerns
natural and synthetic-polymer-based materials, and their recent applications have arisen regarding the production of
in the development of biodegradable e-skin in wearable sensors, robotics, and electronic waste (e-waste), the influence
human–machine interfaces (HMIs). Finally, the main challenges and outlook of e-skin on human health, the safety of
regarding the preparation and application of biodegradable e-skins are criti- wearable electronic devices, costs, and
cally discussed in a near-future scenario, which is expected to lead to the next environmental limitations. These concerns
have encouraged researchers to develop
generation of biodegradable e-skins.
biocompatible, renewable, sustainable, and
biodegradable flexible wearable detection
devices and biosensing platforms.[12–16]
1. Introduction Biological skin regularly regenerates the old superficial layer
of the epidermis with new skin cells during the healing process.
Biological skin is a highly complex organ with an extensive Inspired by this natural degradation cycle, artificial biodegradable
ultrasensitive sensor network that provides simultaneous bio- skin-based electronics should be designed for programmable deg-
sensing, characterization, and differentiation of various stimuli, radation, in contrast to conventional electronic materials. To achieve
such as temperature, pressure, humidity, pain, tactility, and this goal, the development of biocompatible, environmentally
friendly electronic systems that can be used for the fabrication of
biodegradable and sustainable e-skins is important.
M. Zarei, S. G. Lee Various low-cost, nontoxic, renewable, and natural sub-
Department of Chemistry stances and polymer-based materials that can be applied to
University of Ulsan
Ulsan 44610, Korea the development of sustainable, biodegradable e-skins and
E-mail: lees9@ulsan.ac.kr alleviate the environmental and health risks of e-waste mate-
G. Lee, K. Cho rials are available.[17–22] E-waste disrupts the biological activity
Department of Chemical Engineering of microbial enzymes and their metabolisms, which decreases
Pohang University of Science and Technology the resistance and the diversity of soil-based microbial commu-
Pohang 37673, Korea
E-mail: kwcho@postech.ac.kr
nities.[23] In addition, in the human body, the accumulation of
metals and metalloids used in the fabrication of conventional
The ORCID identification number(s) for the author(s) of this article
can be found under https://doi.org/10.1002/adma.202203193. electronics can cause a range of biophysical malfunctions and
diseases, such as liver damage by Cu, behavioral disorders by
DOI: 10.1002/adma.202203193 Pb, and lung cancer and kidney damage by Cd.[24–27]
Adv. Mater. 2023, 35, 2203193 2203193 (1 of 36) © 2022 Wiley-VCH GmbH
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Figure 1. Recent applications, major transduction mechanisms (capacitance, piezoelectricity, and piezoresistivity), and challenges of e-skins. Image for
“Robotics”: Reproduced under the terms of the CC-BY Creative Commons Attribution 4.0 International license (https://creativecommons.org/licenses/
by/4.0).[31] Copyright 2020, The Authors, published by MDPI. Image for “Artificial nerve”: Reproduced with permission.[32] Copyright 2018, American
Association for the Advancement of Science. Image for “Soft robotic”: Reproduced with permission.[33] Copyright 2020, Springer Nature. Image for
“Self-healing”: Reproduced with permission.[34] Copyright 2019, American Chemical Society. Biomedical and Analytical Sciences. Image for “Motion
monitoring”: Reproduced with permission.[35] Copyright 2018, Wiley-VCH. Image for “Tactile sensing”: Reproduced with permission.[36] Copyright
2020, Elsevier B.V. Image for “Pressure imaging”: Reproduced under the terms of the CC-BY Creative Commons Attribution 4.0 International license
(https://creativecommons.org/licenses/by/4.0).[37] Copyright 2020, The Authors, published by Springer Nature. Image for “Smart prosthetics”: Repro-
duced with permission.[38] Copyright 2018, American Association for the Advancement of Science. Trends & Challenges. Image for “Power generation”:
Reproduced with permission.[39] Copyright Elsevier B.V. Image for “Biocompatibility and Biodegradability ”: Reproduced with permission.[14] Copyright
2020, The Authors, published by National Academy of Sciences, USA. Image for “Wireless connectivity”: Reproduced with permission.[40] Copyright
2020, American Association for the Advancement of Science. The hand-to-hand interaction was sketched and inspired by “The Creation of Adam”.
Plant-based materials, such as flowers, wood, and leaves, are rials are desirable for the production of sensitive biodegrad-
favorable candidates for the development of biodegradable elec- able e-skins.[28] In addition, various biodegradable synthetic
tronics because of their abundance, robustness, sustainability, polymers, such as poly(octamethylenemaleate (anhydride) cit-
biocompatibility, availability, and biodegradability. The unique rate) (POMaC), poly(glycerol sebacate) (PGS), and poly(l-lactic
mechanical characteristics and structures of plant-based mate- acid) (PLLA), have been used for the fabrication of flexible
biodegradable wireless sensors.[29,30] The incorporation of such tial for the development of sensitive and affordable e-skins. The
biodegradable materials into flexible electronics and sensors somatosensory system of human skin interprets various tactile
will open new horizons for the development of highly sensitive stimuli and provides the substantial capability to recognize
biodegradable e-skins. objects. It also enables sensory-motor feedback, the discrimi-
This review focuses primarily on the definitions and mecha- nation of textures, and social exchanges.[46,47] The activation of
nisms of transduction in e-skins. First, biologically inspired cutaneous sensory neurons called low-threshold mechanore-
sensations in e-skins are described. The various biodegradable ceptors (LTMRs) is the first step to perceiving innocuous touch
e-skins and their design, fabrication, and integration methods on the skin (Figure 2a–d). The somatosensory system operates
are next discussed. In addition, the most recent breakthroughs, on the basis of the three major functions: proprioceptive func-
developments, and applications of biodegradable e-skins are tions, which are responsible for the perception and control of
highlighted and recent trends in sensors, robotics, and human– the body position, and exteroceptive and interoceptive func-
machine interfaces (HMIs) are summarized. Finally, the limi- tions, which are responsible for perception and reaction to
tations and challenges of biodegradable e-skins are discussed, stimuli originating outside and inside the body, respectively.
and their outlooks and applications are predicted. Herein, the Activation of the primary sensory neurons that reside within
mechanism of action and the current state of biodegradable dorsal root ganglia (DRG) and cranial sensory ganglia is the
e-skins are reviewed, with emphasis on the period of the last first step in somatosensory perception. To decipher harmful
five years; their development into future applications is then stimuli, most DRG neurons are tuned to sense nociceptive and
extrapolated. thermal stimuli. The specific mechanosensitive sensory neu-
rons serve to understand and interpret noxious and innocuous
touch sensations. These specific mechanosensitive sensory
2. E-Skins: Definitions and Mechanisms neurons are classified into two general categories: high-
threshold mechanoreceptors (HTMRs), which react to harmful
of Transduction
mechanical stimuli, and LTMRs, which respond to innocuous
High-performance biosensing via wearable electronics is a mechanical stimulation. The sensory system is tradition-
critical subject in the development of implantable sensors, ally defined as discrete channels or labeled lines that transfer
e-skins, and human–machine interactive electronics.[11,41–43] the cutaneous sensory information from the periphery to the
Various human-inspired emulation systems have been devel- somatosensory cortex. However, anatomical and physiological
oped, including high-resolution cameras, electronic noses, and experiments have shown that sensory integration starts at sub-
high-fidelity stereo systems. However, for the simulation of skin, cortical levels. Currently, researchers can verify that a unique
serious challenges and limitations in providing high sensitivity combination of ion channels, cutaneous LTMR endings, and
and rapid response for the tactile sensing simulation of human central network system circuits is responsible for the tactile
skin remain unsolved. Biological skin comprises several bar- perception on the basis of acute ablation and/or silencing
rier layers, including a primary barrier that prevents the entry of neuronal subtypes and molecular genetics. The skin is
of microbes and viruses and the loss of water and extracellular innervated by complex combinations of LTMRs and HTMRs,
fluid. In addition, skin glands produce acidic secretions, which each with unique physiological profiles and response properties
retard the growth of fungi. Furthermore, in the second barrier, elicited by distinct tactile stimuli.
melanocytes provide efficient protection against the damaging The wetness perception is driven by the thermal sense, spe-
effects of ultraviolet radiation. Specific skin functions such as cifically the cold thermosensitivity of biological skin.[48] Ther-
protection, temperature regulation, water balance, sensory recep- mosensitivity is the primitive form of skin wetness perception,
tion, production of hormones and vitamins, and material absorp- which includes the water interaction and evaporation from
tion are induced by skin homeostasis, which is generated by a the skin surface that leads to the heat transfer in the form of
constant turnover of the epidermis and distinct stem cells.[44,45] evaporative cooling, hence cold sensations in biological skin.
The ability to distinguish and simultaneously sense multiple The moisture interaction with the skin surface includes two
mechanical forces, temperature, and humidity provides a physi- paths of skin deformation (mechanical component) and con-
ological balance between the human body and the ambient ductive and evaporative heat transfer (thermal component)
environment. Inspired by the biological skin’s somatosensory (Figure 2e).[48] Any changes in the mechanics and tempera-
system, various physical transduction mechanisms in e-skins ture profile of skin trigger the activation of mechano-sensitive
have been introduced, including capacitance, piezoresistivity, and temperature-sensitive neurons, that is, thermoreceptors
and piezoelectricity. Recently, self-healing and self-powered elec- and mechanoreceptors that convey afferent peripheral sensory
tronics, which are desirable for the fabrication of next-generation inputs. Then, the somatosensory neural system integrates
multifunctional ultrasensitive e-skins, have been introduced. these peripheral inputs arising from mechanosensory and ther-
This section discusses the sensing system of biological skin and mosensory sources to trigger the perception of skin wetness.
various mechanisms of transduction in e-skins. Biological skin is composed of a unique combination of var-
ious mechanical and sensory characteristics and networks una-
vailable in conventional electronics. In this case, to mimic the
2.1. Mimicry of Skin: A Biologically Inspired Sensation biological skin characteristics, scientists must understand the
somatosensory functions precisely and develop novel materials
Understanding the sensing architecture and key elements that and approaches to fabricate the most efficient and affordable
influence the sensory characteristics of natural skin is essen- skin-inspired electronics.
Figure 2. The somatosensory system of biological skin. a) Schematics of the biological skin mechanoreceptors organization and their related optimal
stimulus. b) Postulated LTMR activity map in response to common tactile stimuli, *NR: Not reported. a,b) Reproduced with permission.[46] Copyright
2013, Elsevier. c) LTMR end organs of glabrous skin. Reproduced with permission.[49] Copyright 2014, American Association for the Advancement of
Science. d) Merkel-cell inputs in touch reception. Skin deformation opens mechanotransduction channels in slowly adapting type I (SAI) afferents (1),
which causes the firing of the action potential at the beginning of dynamic stimuli (2). Deformation of the skin actuates the Piezo2-dependent mecha-
notransduction channels of Merkel cells (3), which generates calcium entry through the calcium channels (CaV) (4) and neurotransmitters release (5)
that promote the sustained firing of action potentials (6). Reproduced with permission.[50] Copyright 2014, Springer Nature. e) Main mechanisms for
the sensory integration of human skin wetness perception including physical, biophysical, and neurophysiologic mechanisms. Reproduced with permis-
sion.[48] Copyright 2018, Elsevier B.V.
2.2. Mechanisms of Transduction stress of 13.3 kPa was applied, representing an 85-fold enhance-
ment in performance compared with that of native wood, with
Efficient wearable electronics should sense various mechanical stable performance for ≥600 cycles. This nanogenerator system
deformations such as shear forces, pressure, twist, and strain. can be integrated into a wearable motion-monitoring device
During signal transduction, an external stimulus is translated and can be produced from a single wood sponge or large-scale
into one specific analog electronic signal. In general, con- prototype (for powering an LED light and an LCD screen) with
ventional transduction methods can be classified into piezo- the enhanced output produced from 30 wood sponges.
electricity,[51,52] piezoresistivity,[53,54] and capacitance.[55,56] Other The biodegradable PLLA has also been used to fabricate the
methods such as triboelectric, wireless, and optical approaches piezoelectric flexible wearables and flexible electronics. In 2020,
have been used for the development of high-performance Curry et al.[14] described a strategy for the efficient fabrication
e-skins for various sensing and HMI applications (Table 1).[57–60] and electronic integration of biodegradable and biocompatible
In this section, details of recently reported transduction mecha- piezoelectric PLLA nanofibers (Figure 3a). Their reported mate-
nisms and related applications are discussed, with emphasis on rial exhibited stable and highly controllable piezoelectric perfor-
biodegradable e-skins. mance, which can be used in implantable devices such as pres-
sure sensors and biodegradable ultrasonic transducers appli-
cable to blood–brain barrier opening and drug delivery. In addi-
2.2.1. Piezoelectricity tion, Hanani et al.[96] prepared a Pb-free, biocompatible, and
flexible piezoelectric nanogenerator (BF-PNG) via a core–shell-
Piezoelectricity is defined as the linear interaction between elec- structured Ba0.85Ca0.15Zr0.10Ti0.90O3 filler with a polydopamine
trical and mechanical quantities. Mechanical deformation of (PDA) layer and a biodegradable polylactic acid (PLA) matrix.
certain materials under an applied mechanical load produces Under gentle finger tapping, the designed BF-PNG generated
a macroscopic variation of electric polarization, which can be an open-circuit voltage of 14.4 V and a short-circuit current
measured as an electric voltage or electric charge related directly of 0.55 µA. The prepared BF-PNG exhibited high mechanical
to the applied mechanical force (Figure 1). Dipole moments can robustness, durability, and stability during 14 000 cycles after
be induced by the deformation of noncentrosymmetric crys- 1 year of aging. In addition, under gentle finger tapping, the
tals[89] or certain porous dielectric materials.[90] Inorganic rigid prepared BF-PNG was used to drive a 1 µF capacitor to store
piezoelectric materials and flexible energy-harvesting polymers 3.92 µJ of energy within 115 s.
have been used to develop tactile sensors, health monitoring Biobased piezoelectric materials including collagen, amino
devices, and wearable electronics. Piezoelectric materials with an acids, cellulose, and peptides have been studied comprehensively
asymmetric atomic crystal structure and stable polarization, such because of their abundance, biocompatibility, biodegradability,
as BaTiO3 (BTO), Pb(ZrxTi1−x)O3 (PZT), and ZnSnO3, have been low-cost, and simple processing.[97,98] In 2020, Hosseini and
used extensively.[91] However, these ceramic materials are unsuit- co-workers[77] prepared flexible biodegradable pressure sen-
able for the development of wearable electronics because of their sors based on free-standing and biodegradable β-glycine–chi-
rigidity. Among them, PZT is one of the most widely used piezo- tosan (β-Gly/CS) piezoelectric films. The piezoelectric β-Gly/
electric materials; however, PZT suffers limitations, including CS generated a 190 mV output voltage under 60 kPa pressure,
harsh synthesis routes, toxicity, and poor mechanical character- with a sensitivity of 2.82 ± 0.20 mV kPa−1. The pressure sensor
istics. These limitations hinder the widespread use of PZT for remained stable after 9000 cycles. The authors claimed that the
biomedical applications such as implantable medical devices piezoelectricity of β-Gly/CS could be used to generate a voltage
and give rise to environmental pollution challenges related to its from biological deformation to provide electrical stimulation for
disposal. In this regard, the fabrication of biodegradable piezo- tissue repair/regeneration and wound healing because of the
electric materials is important for various applications, such as migration of cells toward the wounded area under the influence
mechanical energy harvesters and flexible wearable sensors. of an external electric field (as low as 12.5 mV mm−1), which
Piezoelectric nanogenerators (PENGs)[92–95] have been accelerates the healing process.[99] In another study,[91] a bio-
studied extensively for the efficient conversion of mechanical degradable β-rich chitin polymer from squid pen material was
energy to electric energy. Dahiya et al.[51] developed a low- prepared and used to develop a flexible transparent piezoelectric
voltage graphene field-effect transistor (GFET) pressure sensor transducer (Figure 3b). The chitin film exhibited piezoelectric
based on biocompatible and biodegradable piezoelectric mate- characteristics, with an output current density of 177 nA cm−2
rials. The device was composed of a biodegradable β-glycine/ for 5000 cycles under 100 kPa pressure. The prepared chitin
chitosan composite based on a metal–insulator–metal (MIM) material was digested by the chitinase enzyme without the gen-
structure connected to a GFET. The device exhibited a sensi- eration of toxic byproducts. In 2021, a fully biodegradable fer-
tivity of 2.70 × 10−4 and 7.56 × 10−4 kPa−1 in the pressure ranges roelectric bimodal sensing e-skin was developed based on edible
5–20 and 20–35 kPa, respectively. The device could be operated porcine skin gelatine (Figure 3c) with a zero-waste footprint.[100]
at a very low operation voltage (50 mV), which is beneficial for The interlocked microdome microstructures and molecular
the development of energy-efficient large-area e-skins. In 2020, properties of gelatine induced the polarization confinement and
Sun et al.[15] developed a compressible, biocompatible, low-cost, ferroelectric characteristics, resulting in a piezoelectric coeffi-
and biodegradable piezoelectric nanogenerator based on a wood cient (d33) of ≈24 pC N−1, which was 6 times higher than planar
sponge. Because of the increased compressibility of the wood gelatine. The developed self-powered e-skin exhibited low LOD
sponge, this wood nanogenerator produced an instantaneous (≈0.005 Pa) and high-pressure sensitivity (≈41 mV Pa−1). The
voltage of 0.69 V and a current of 7.1 nA when a relatively small authors suggested this e-skin could sense the surface texture,
Table 1. Material development, performance, transduction mechanism, and applications of developed sensors and e-skins.
Materials Mechanism Sensitivity & Performance Range Ref Stability & Response time Application
−1
Graphene, Porous Nylon, PDMS Capacitive 0.33 kPa <1 kPa [61] >1000 cycles <20 ms Flexible tactile devices, health monitoring,
motion detection
Polyacrylamide (PAM)/alginate Capacitive 3.19 kPa−1 0.025–20 kPa [62] > 1400 cycles < 220 ms Motion monitoring, HMI, soft robotics, AI
hydrogel
PDMS, Poly(ethylene tere- Capacitive 14.268 kPa−1 (<0.7 kPa), <30 kPa [63] 10 000 cycles <50 ms Disease diagnosis, monitoring, wearable
phthalate) (PET), Ti/Au 0.032 kPa−1 (0.7−40 kPa) devices, prosthetics
Graphene, PDMS, PET, SU-8 Capacitive 6.55 kPa−1 (0–16 kPa), 1.15% 0–30 kPa [64] 500 cycles 70 ms Tactile sensing, portable, wearable devices,
kPa−1 (16–30 kPa) large-scale touch screens
Silver nanofibers, Silver Capacitive ≈1.78 × 10−3 kPa−1 0–1.6 MPa [65] 15 000 cycles 32 ms Tactile and skin temperature sensors
nanowires, PEDOT:PSS, Indium (<350 kPa), 9.65
gallium zinc oxide × 10−5 kPa−1 (>350 kPa)
Silicone, CNT, Polyhydroxy- Capacitive 0.19 ± 0.07 kPa−1 (P < 0–100 kPa [66] 30 000 cycles millisecond Robotics with tactile feedback,
butyrate–polyhydroxyvalerate 1 kPa), 0.10 ± 0.01 kPa−1 range personalized medicine, surgery
Polyurethane (1 < P <10 kPa), 0.04 ± 0.001
kPa−1 (10 < P < 20 kPa)
Polystyrene, PDMS, Au Capacitive 0.815 kPa−1 0−50 N [67] 38 ms E-skins, wearable biomedical devices,
robotics
Bionic micropatterned PDMS Capacitive 1.2 k Pa−1 <10 kPa [68] 100 000 cycles 36 ms Flexible tactile sensors, health monitoring,
soft robots, motion detection
AgNWs, PDMS, PEDOT:PSS Capacitive 0.07–74 N 0.78–10.3 MPa [69] >3500 cycles <50 ms Joint rehabilitation, soft robotic fields
CNTs, Thermoplastic Piezoresistive 136.8 KPa−1 <200 Pa [53] 1000 cycles Health monitoring, motion detection
elastomer (TPE)
Tissue paper, AgNWs, Nanocel- Piezoresistive 1.5 kPa−1 0.03−30.2 kPa [70] 90 ms Disposable pressure sensors, paper-based
lulose paper flexible electronic devices
PGS, MWCNTs, NaCl Piezoresistive 0.12 ± 0.03 kPa−1, 8.00 ± ≤8 kPa [16] >200 000 cycles ≤20 ms Wearable devices, motion monitoring,
0.20 kPa−1 recreation, tissue engineering
Graphene, PDMS Piezoresistive GF: 2.87−8.77 0−50% [54] 36 000 cycles & 100 cycles Pressure sensor, Personalized health
monitoring, human motion detection
AgNWs, Reduced graphene Piezoresistive 5.8 kPa−1 < 5 kPa [61] >10 000 29.5 ms Detection of pulse waves, smart wearable
oxide (rGO) electronics, human motions monitoring
Poly(vinyl alcohol-co-ethylene), Piezoresistive 2.79 kPa−1 - [71] 3506 cycles 3 ms Monitoring of large-area spatial pressure
Polypyrrole, Polyolefin distribution, wearable intelligent interactive
elastomer devices
Aligned carbon nanotubes/gra- Piezoresistive 19.8 kPa−1, <0.3 kPa [72] 35 000 cycles <16.7 ms Wearable electronics
phene, microstructured PDMS
PET, Liquid metal (eGaIn, Piezoresistive ((2−20) × 10−3 kPa−1) 2−400 kPa [73] 500 cycles Tactile Sensor
Galinstan)
PDMS, MWCNT Piezoresistive −1.10 kPa−1 <21 kPa [74] 2000 cycles 29 ms Tactile sensor
SWCNT, Polyethylene, PDMS Piezoresistive −3.26 kPa−1 0−300 Pa [75] 5000 cycles 200 ms Tactile sensor, robot skins and haptic
perception
PDMS, SWNTs, Silk piezoresistive 1.80 kPa −1 0.6 Pa <1.2 [76] >67 500 cycle <10 ms Wearable electronic, Monitoring of
kPa physiological signals
β-Glycine, Chitosan Piezoelectric 2.82 ± 0.20 mV kPa−1 5−60 kPa [77] >9000 cycles <100 ms Wearable biomedical diagnostics
Carbonized electrospun polyac- Piezoelectric 1.44 V·N−1 0.15−25 N [78] 60 000 cycles Human-computer interactive, wearable
rylonitrile/barium titanate sensing devices, physiological sensing
Polycarbonate track-etched, Piezoelectric 0.21 V kPa−1 <1 kPa [79] 20 ms Mimicking cutaneous mechanoreceptors
Polyaniline (PANI), Au/polyvi-
nylidene fluoride (PVDF)
Pb[Zrx,Ti1−x]O3, PET Piezoelectric 0.018 kPa−1 1–30 kPa [80] 5000 cycles 60 ms Arterial pulse monitoring
PVDF/ZnO nanofibers Piezoelectric 4.4 mV deg−1, 0.33 V kPa−1 44˚ to 122˚, [81] 5000 cycles 76 ms & 16 ms Interactive HMI, physiological signal
1–30 kPa monitoring, gesture sensing
PDMS, PVDF Piezoelectric 1.5 × 10−5 V mN−1. 8–24 N [82] 1.4 × 104 cycles Self-powered human motion sensors
Table 1. Continued.
Materials Mechanism Sensitivity & Performance Range Ref Stability & Response time Application
−1
AgNW, Silicone Triboelectric- 34 mV Pa <1.7 kPa [83] 5800 cycles 90 ms Tactile Gesture Sensing, HMI, AI, soft
Photonic robotics
PEDOT:PSS, PDMS Triboelectric 0.08 kPa−1 (2–60 kPa), 0.008 2–160 kPa [84] 200 cycles 227 ms & 35 ms HMI, e-skins, soft robotics, wearable
kPa−1 (60–160 kPa) electronics
Graphene, Poly(ethylene Triboelectric 0.04–1.63 kPa−1 <100 kPa [85] 10 000 cycles <3 ms Soft robotics, prosthetics, HMI
naphthalate),
Poly(tetrafluoroethylene)
PDMS, Indium tin oxide, Triboelectric 2.82±0.18 V MPa−1 0.3–612.5 kPa [86] 40 ms Tactile sensing, display, wearable electronics,
Polyester, PET artificial skins, IoT
PDMS, Pectin Triboelectric 3.627 kPa−1 (0–8 kPa) 1.264 1–80 kPa [87] 5000 cycles 40 ms Wearable electronics, internet of healthcare,
kPa−1 (8–80 kPa) LOD≈5Pa low power consumption applications
Siloxene-polyvinylidene fluoride Triboelectric 12.062 VkPa−1 (<3 kPa) 2.58 0–25 kPa [88] 60 000 cycles Self-powered IoT, smart tactile-based
VkPa−1(3–25 kPa) authentication platforms
Figure 3. Biodegradable piezoelectric sensors and e-skins. a) Piezoelectric PLLA nanofibers for the fabrication of biodegradable implanted piezoelectric
devices. Reproduced with permission.[14] Copyright 2020, The Authors, published by National Academy of Sciences, USA. b) Photograph of transparent
chitin preparation and biodegradability. Reproduced with permission.[91] Copyright 2018, Elsevier, B.V. c) Biodegradable ferroelectric edible porcine gela-
tine e-skin. Reproduced under the terms of the CC-BY Creative Commons Attribution 4.0 International license (https://creativecommons.org/licenses/
by/4.0).[100] Copyright 2021, The Authors, published by Wiley-VCH.
Figure 4. Biodegradable piezoresistive sensors and e-skins. a) Fabrication and working mechanism of the KC/SPP/KC (KSPPK) e-skin. Reproduced
with permission.[102] Copyright 2021, Wiley-VCH. b) Mechanism and performance of all-paper piezoresistive e-skin. Reproduced with permission.[70]
Copyright 2021, American Chemical Society.
spatially resolved pressure, and temperature, due to the large a detector.[101] Wearable, flexible piezoresistive sensors have
pyro/piezoelectric coefficients. The developed biodegradable attracted attention as HMIs in biomedical engineering and
e-skin nanogenerator was able to sense the touch and tempera- materials science because of their simple device design, flex-
ture variations in the surroundings, which enabled dexterous ibility, sensitivity, and efficient signal reading. Natural materials
manipulation of objects. The highly enhanced ferroelectric and and biopolymers are appropriate candidates for the develop-
piezoelectric behavior of gelatine microdome film was attrib- ment of biodegradable piezoresistive e-skins. In 2021, Xu
uted to the increased molecular packing, which was induced by et al.[102] developed a biodegradable, breathable piezoresistive
spatial confinement within the microdome structure. Also, the e-skin by constructing a 3D network structure based on silk
gelatine microdome exhibited a higher amount of crystallinity fibroin (SF)/poly(lactic-co-glycolic acid) (PLGA)/polyaniline
(29%) compared to the planar structure (15%), which contrib- (PANI) (SPP) that encapsulated with the biological polysac-
utes to the enhanced piezoelectric performance of microdomes. charide κ-carrageenan (KC) (Figure 4a). In this device, poly-
aniline acted as an active conductive filler in a 3D conductive
network, while SF and PLGA were utilized for the formation of
2.2.2. Piezoresistivity a network for carrying conductive materials. This piezoresistive
e-skin exhibited a wide linear detection range (165.3 kPa) and
In piezoresistive materials, variations of force transduction good sensitivity (2.54 kPa−1), which were attributed to the sub-
result in changes in resistance that can be measured using stantial deformation of the SPP network and enhanced contact
between fibers under applied pressure. In one study, an all candy, and a stretchable sensor, confirming the reconfiguration
paper-based piezoresistive (APBP) pressure sensor was intro- capability of the sensor. A biodegradable capacitive pressure
duced based on a nanocellulose paper (NCP) as a bottom sub- sensor was developed for the measurement of the atrial blood
strate for printing electrodes, a tissue paper coated with silver flow in both contact and non-contact modes (Figure 5b).[30] The
nanowires (AgNWs) as a sensing material, and NCP as a top capacitive sensing platform was based on fully biodegradable
encapsulating layer (Figure 4b).[70] The APBP pressure sensor materials including Mg as an electrical interconnect, PGS as a
exhibited a sensitivity of 1.5 kPa−1 (0.03–30.2 kPa), ultralow dielectric layer, POMaC and polyhydroxybutyrate/polyhydroxy-
energy consumption (≈10−8 W), a low working voltage (0.1 V), valerate (PHB/PHV) as packaging layers, and PLLA as an insu-
and a short response time (90 ms). This sensor can be applied lation spacer. The working mechanism was based on arterial
as a soft e-skin and used to monitor physiological signals such pulsation that caused a variation in vessel diameter, which was
as finger touch, arterial heart pulses, and pronunciation. One of measured by the capacitive pulse sensor mounted around the
the advantages of this sensor is that all the sensor components artery.
are paper-based materials, resulting in a biodegradable sensor In 2019, a flexible biodegradable protein-based capacitive
that can be disposed of by incineration. The bacterial cellu- e-skin was introduced based on the integration of SF film with
lose and chitosan were used by Huang and co-workers[103] to Ag nanofibers, which was capable of detecting pressure and
prepare compressible, flexible, and electrically conductive bio- strain with a wide monitoring window ranging from 35 Pa to
mass-based aerogels for the development of piezoresistive sen- 700 kPa.[110] The reported e-skin exhibited biocompatible char-
sors. Their PANI/bacterial cellulose/chitosan (BC/CH) aerogel acteristics such as gas air/water-permeable and inflammation-
exhibited high mechanical strength, low density, good electrical free properties, which confirmed the applicability of this e-skin
conductivity, and the ability to recognize a wide range of pres- for long-term lamination onto human skins (Figure 5c). Con-
sures. These piezoresistive pressure sensors based on PANI/ sidering the biocompatible and biodegradable features, the
BC/CH aerogels could detect a low compressive stress (32 Pa) reported e-skin was promising to find potential applications in
and provide cycling stability and a sensitivity of 1.41 kPa−1. skin-attachable electronics and implantable medical platforms.
Biodegradable polymers such as PGS are suitable for the Recently, Gunal et al.[111] prepared transparent and stretchable
development of flexible and wearable electronics that mimic poly(ethylene glycol-sebacate) elastomers with capacitive and
the properties of human biological skin because of their out- self-healing characteristics that could be used in wearable sen-
standing mechanical properties and high elastic moduli.[104] sors, tactile sensors, and soft electronics. The US Food and
Sencadas et al.[16] reported sensitive and biodegradable porous Drug Administration (FDA) has approved the use of biocom-
piezoresistive sensors based on PGS, multiwalled carbon nano- patible and biodegradable sebacic acid (SA) and poly(ethylene
tubes (MWCNTs), and sodium chloride (NaCl). This sensor glycol) diglycidyl ether (PEGDGE) for the preparation of this
demonstrated detection at low pressures (100 Pa), a short elastomeric material. The resultant materials exhibited high
response time (≤20 ms), long lifetime and stability (>200 000 stretchability and transparency, as demonstrated by their capac-
cycles), and high force sensitivity (≤4 mN). Single linear itive and self-healing behaviors, even at ambient temperature.
behavior over an extensive range of pressures (≤8 kPa) and an
increase in sensitivity from 0.12 ± 0.03 to 8.00 ± 0.20 kPa−1 was
achieved after 8 weeks in a medium of simulated body fluid. 2.2.4. Other Mechanisms
The conventional transduction mechanisms offered advantages

2.2.3. Capacitance but exhibited specific limitations for application in hybrid and
complex sensing platforms (Table 2), which encouraged the
The capacitance in a simple capacitor is described as the ability scientific society to develop new types of strategies including
to store an electrical charge (Figure 1).[105] The development of triboelectric, multimodal, optical, temperature, humidity,
e-skins based on capacitive transduction is expanding because chemomechanical, wireless, and acoustic sensing strategies
of their high sensitivity, rapid response, simplicity, low limit to remedy the limitations of conventional mechanisms. Some
of detection, and low drift.[106,107] In general, a capacitive e-skin recently developed approaches that are distinct from conven-
is composed of a dielectric layer sandwiched between flexible tional transduction methods have been utilized for the fabri-
electrodes. When the sandwiched structure is compressed, cation of biodegradable e-skins. For example, a triboelectric
the capacitance changes with the electrodes’ distance. Dif- nanogenerator (TENG) converts different mechanical stimuli at
ferent materials, including foams,[108] elastomers,[107] and poly- both low/high frequencies into electricity via contact electrifi-
mers,[61] have been used as the dielectric layer in capacitive cation.[112] TENGs have the advantages of being highly flexible,
sensors. In one study, Zhao et al.[109] introduced an all-paper, lightweight, structurally adaptable, and stable, and the suc-
reconfigurable, and shape-designable capacitive pressure/prox- cessful application of TENGs in energy-harvesting e-skins has
imity sensor using polypyrrole printer paper for the electrode/ been demonstrated.[113–115]
encapsulation layer and tissue paper as the dielectric layer Triboelectricity: Triboelectrification is a natural phenom-
(Figure 5a). The authors reported that the sensor exhibited a enon, which creates static polarized charges in two originally
superior sensitivity of 0.96 kPa−1 at <1.76 kPa and 0.09 kPa−1 at uncharged bodies.[126] This process is one of the fundamental
1.76–22 kPa. In addition, the reported capacitive sensor could principles of TENG-based systems, which generally includes
be fabricated into sensors with a 2D shape or freestanding 3D two different materials that are assembled in direct con-
structure, including a 3D smart box, a 2D braille keyboard, 3D tact with each other. Due to the contact electrification effect,
Figure 5. Biodegradable capacitive sensors and e-skins. a) Schematic of all-paper pressure/proximity sensor. Reproduced with permission.[109] Copy-
right 2021, American Chemical Society. b) Flexible arterial-pulse capacitive sensor.[30] Copyright 2019, Springer Nature. c) Protein-based capacitive
e-skin. Reproduced with permission.[110] Copyright 2019, Wiley-VCH.
opposite static charges appear on the surfaces of the materials regarded as representative triboelectric materials for positively
in direct face-to-face contact. By separation of contact bodies, charged and negatively charged films, respectively. The highest
the charges flow between two attached electrodes through an triboelectric outputs of this TENG were ≈ 20 V and ≈ 0.4 µA and
external circuit, which generates a potential difference.[127] The the maximum power density was ≈ 5.6 mW m−2 at 60 MΩ. In
development of TENGs based on electrostatic induction and 2020, Ma et al.[131] developed a flexible fish-bladder-film-based
triboelectrification has been proven to be a promising strategy TENG (FBF-TENG) for e-skin applications. In this sensor, the
for the fabrication of self-powered e-skins because of its high biocompatible and biodegradable natural material was used as
efficiency for the conversion of vibration energy to electrical a triboelectric layer (Figure 6b). The FBF-TENG demonstrated
energy.[128] Recently, several types of TENG-based biodegradable an output current density and charge density of 4.56 mA m−2
flexible skin-inspired sensors and e-skins have been developed and 25 µC m−2, respectively. Kar et al.[132] developed a flex-
for the perception of various mechanical stimuli.[126,129] ible, biocompatible, and biodegradable energy harvester using
Animal-derived compounds have been used in the devel- chicken-feather fibers. These fibers are an abundant biowaste
opment of TENG-based wearable devices, sensors, and elec- material, with excellent mechanical characteristics and a high
tronics. The hyaluronic acid (HA) is a biopolymer and the main surface-to-weight ratio. Under the biomechanical pressure of
component of the mammalian extracellular matrix, which has a a finger (0.13–0.31 MPa), the developed device exhibited an
linear disaccharide polymeric chain. Recently, a biodegradable output voltage of 10 V, power density of 6 µW cm−2, and current
and biocompatible TENG was developed based on a HA density of 1.8 mA cm−2. The good piezoelectric performance of
hydrogel film and 1,4-butanediol diglycidyl ether (BDDE) as this device was attributed to the constituent hydrogen bonds of
a cross-linker (Figure 6a).[130] The TENGs based on pure HA the keratin structure in the chicken-feather fibers (1.6 ≤ d33 ≤
or crosslinked HA hydrogel films were prepared with various 2.1 pC N−1). The disulfide bonds of the chicken-feather fibers
counterparts, including mica film and PTFE, which were provided mechanical robustness.
Table 2. Advantages and disadvantages of capacitive, piezoresistive, fication. Wu et al.[134] introduced a fully biodegradable TENG
and piezoelectric transduction mechanisms. (FBD-TENG) based on natural substances (Figure 6c). In their
work, water droplets acted as both tribomaterials and conduc-
Transduction Advantages Disadvantages Ref tive top electrodes, leaf cuticles were used as both dielectric and
Mechanism
triboelectric materials, and conductive leaf tissues were used
Piezoelectric High sensitivity Poor spatial resolution [116–120] as bottom electrodes. Consequently, the impact of droplets not
High-frequency response Charge leakages only generated surface charges on the dielectric surface but
Wide dynamic range Non-effectiveness in static
also bridged the disconnected components into a single closed-
environments
loop electrical system, thereby producing electricity. With this
Piezoresistive Low cost Non-reproducibility [121–123] device, the current and voltage of 4 µA and 1 V were achieved
High sensitivity Hysteresis
as a result of water impacting the leaf surface of Mytilaria lao-
Simple design High power consumption
sensis. Considering various plants and rich water droplets in
High spatial resolution
natural ecosystems, the reported strategy could be beneficial for
Capacitive Large dynamic range Hysteresis [28,124,125]
energy-harvesting and plant-based sensing in home gardens,
High sensitivity Stray capacitance
forests, islands, and remote resource-limited settings.
Fast response Complex measurement
Less drift circuit
Optical and Photonic Sensing: The optical and photonic
Low LOD Elements cross-talks sensing platforms have been widely employed in the develop-
Simple design Noise susceptibility ment of biomedical and analytical sensing devices because of
Temperature independent their high accuracy, efficiency, and versatility.[135] The modi-
fication of physicochemical characteristics such as electronic
bandgap, dielectric behavior, electrical conductivity, and struc-
A cellulose-based TENG with improved polarity and tural design, can improve the light response and the detection
hydrophobicity was prepared by chemical functionalization performance in biodegradable optical sensors and e-skins.
to control the surface polarizability and hydrophobicity in In this regard, the application of natural and synthetic biode-
moisture-resistant cellulose nanofibrils (CNs).[133] Triethoxy- gradable materials and waveguides such as cellulose,[136,137]
1H,1H,2H,2H-tridecafluoro-n-octylsilane (also known as per- chitin,[138] silk,[139] PLA,[140] and PLLA[141] have been reported.
fluorooctyltriethoxysilane, PFOTES) was used to modify the The chitin nanofiber (ChNF) paper was introduced for the
functional groups on the CN surface, which enhanced the tri- development of biodegradable, transparent, and miniatur-
boelectric charge density, hydrophobicity, and surface polarity ized optical sensing platforms by embedding/immobilizing
of the CNs. The short-circuit current in the PFOTES-CN-based plasmonic materials (e.g., Au and Ag nanoparticles), photo
TENG was double that in the CN-based TENG prior to modi- luminescent nanoparticles (e.g., carbon dots) along with
Figure 6. Triboelectric transduction mechanisms in biodegradable e-skins. a) Schematic of HA-TENG working principle. Reproduced with permis-
sion.[130] Copyright 2021, Elsevier B.V. b) The FBF-TENG device charged by the FBF-TENG. Reproduced with permission.[131] Copyright 2020, American
Chemical Society. c) Schematic and working mechanism of FBD-TENG. Reproduced with permission.[134] Copyright 2020, American Chemical Society.
colorimetric reagents (e.g., curcumin and dithizone).[138] The solution (67 days) in a 1% saline solution, while the authors
biodegradable synthetic polymers such as PLLA were used reported the loss of stable electrical operation after about 1
as biodegradable and implantable optical fibers, which were day. Furthermore, using a dissolvable zinc wire, the Bluetooth
integrated into the sensing platform, due to their high flex- operation was achieved on this platform. Another hybrid bio-
ibility and optical transparency.[141] The PLGA- and PLLA-based degradable and bioresorbable optical sensing platform for
polymers exhibited desirable features including ideal flexibility, monitoring pressure and temperature was developed by Shin
ease of fabrication, and controllable degradability, which can and co-workers.[150] The developed device was composed of
be used for the fabrication of various types of biodegradable single-crystalline Si nanomembranes (Si NMs), thermally
e-skins. However, the natural biodegradable materials (e.g., silk) grown silicon dioxide layers, amorphous silica adhesion layers,
and synthetic polymers (e.g., PLGA) usually suffer from limited a silicon slab with a square cavity geometry, and PLGA fibers
tunability for key mechanical, optical, and degradation proper- (Figure 7b). The temperature sensing mechanism in this device
ties. To remedy these shortcomings, other natural candidates was attributed to the coupling of the light into the noncavity
including the family of citrate-based biodegradable elastomers regions of the device. Thus, the developed temperature sensors
have been introduced because of their tunable elastic moduli relied on the temperature-dependent refractive index of silicon
ranging from tens of Pa to MPa, programmable degradation for temperature sensing. The authors suggested their reported
rates ranging from a few days to over a year, ultrafine tuning platform could establish a route for the fabrication of magnetic
of refractive index, and multifunctionality including fluores- resonance imaging (MRI)-compatible and entirely bioresorb-
cent and adhesive compounds.[142] Recently, hybrid dual-mode able pressure and temperature sensing platforms.
optical sensing strategies were proposed for the development Humidity Sensing: Humidity sensing platforms have been
of biodegradable e-skins. For example, Tang et al.[143] developed studied extensively for environmental monitoring systems,
a highly flexible and transparent wood-based e-skin with optical food packaging, Internet of Things (IoT) solutions, industrial
and capacitive dual-mode sensing characteristics. The reported processing, and agricultural processing.[151] However, in bio-
e-skin could be used for curated mapping of the spatial distri- medical science, the application of humidity sensing is limited
bution of static and dynamic pressures through optical sensing. to respiration monitoring.[152,153] In this regard, an entirely bio-
The dual-mode sensing mechanism was based on capacitance degradable device for monitoring human breathing states was
variations under external pressures as a function of distance introduced, which satisfied the major requirements including
changes between electrodes. In addition, under external pres- rapid response time, cyclic stability, high sensitivity, and sen-
sure, the ZnS:Cu phosphor particles exhibited luminescence sitive discrimination of humidity stimuli.[154] The reported
through electro-optical conversion, providing the hybrid dual- bioprotonic device was developed from natural polysaccharide
mode sensing functions for the e-skin.[143] materials which could be decomposed easily in a natural envi-
Temperature Sensing: Continuous and precise monitoring of ronment (Figure 7c). The current of the device was increased
body temperature is essential for healthcare management and by the formation of hydrogen bond networks between the
timely disease diagnostics. In this regard, a variety of high- water and polysaccharides in the polysaccharide films. In addi-
performance temperature sensors and e-skins have been devel- tion, more proton-conducting hydrogen bonds were formed
oped for application in different biomedical settings.[144] Most because of higher water absorption, which led to the formation
of the reported temperature-sensitive e-skins are not biodegrad- of 3D networks that protons could move through these chains
able or even environmentally friendly. Hence, it is necessary to via Grotthuss-type mechanisms.[155] This proton conduction
develop biodegradable and biocompatible platforms that can phenomenon is ubiquitous among biomacromolecule-based
be easily discarded in a natural environment without harmful materials. Another biodegradable humidity sensing platform
byproducts or can be safely resorbed inside the human organs. was proposed based on poly(vinyl alcohol) (PVA)–starch–Y2O3
Various natural biopolymers were reported for the fabrication nanoparticle nanocomposites.[156] In the reported system, Y2O3
of flexible temperature sensing platforms with controllable nanoparticles played an important role in sensing perfor-
biodegradability.[145] Among them, silk proteins were used for mance. The increase of Y2O3 nanoparticle loading increased
the development of ionotronic skins,[146] or all-silk dual-mode the optical conductivity and electrical conductivity because of
e-skin for simultaneous temperature-pressure detection.[147] A an increase in localized stages of bandgaps, absorption coeffi-
biodegradable, transparent, conformal, and fully organic flex- cient, and number of charge carriers, respectively. The cellulose
ible silk/poly(3,4-ethylenedioxythiophene):poly(styrene sul- nanofibers are also another candidate for the development of
fonate) (PEDOT:PSS) platform was reported for temperature humidity and moisture sensing platforms. A transparent and
sensing.[148] The developed system was based on the photo fully biodegradable cellulose nanofiber–PEDOT:PSS moisture
active SF substrate and the photoactive silk sericin–PEDOT:PSS sensor was reported with a wide operation range from 20% to
conductive ink. The reported flexible sensor exhibited high 85% relative humidity, where cellulose nanofiber film acted as
sensitivity and full degradation after 10 days under proteolytic the sensing layer.[152] The sensing mechanism of the reported
conditions. In one study, Salvatore et al.[149] described a biode- humidity sensor was attributed to the water absorption by cel-
gradable and highly deformable temperature sensor based on lulose nanofiber films. The water molecule could modify the
biodegradable components including Mg, SiO2, Si3N4, and a electrical permittivity of sensing materials and change the
compostable flexible polymer such as Ecoflex (Figure 7a). The impedance of the humidity sensor.
reported device exhibited continuous performance with a 10 ms Wireless Sensing: In wireless transduction platforms, the wire-
response time in folded, crumpled, and stretched conditions. less operation was achieved by near-field coupling between
In addition, the device could be tuned for morphological dis- a resonant sensor and an external antenna.[157] The resonant
Figure 7. Biodegradable temperature, pressure, and humidity sensing platforms. a) Schematic, structure, and application of biodegradable tempera-
ture sensors. Reproduced with permission.[149] Copyright 2017, Wiley-VCH. b) Structure of bioresorbable and biodegradable temperature and pressure
sensing platform. Reproduced with permission.[150] Copyright 2019, American Association for the Advancement of Science. From ref. [150]. © The
Authors, some rights reserved; exclusive licensee AAAS. Distributed under a CC BY-NC 4.0 license http://creativecommons.org/licenses/by-nc/4.0/.
Reprinted with permission from AAAS. c) Structure of biodegradable polysaccharide humidity sensor. Reproduced under the terms of the CC-BY
Creative Commons Attribution 4.0 International license (https://creativecommons.org/licenses/by/4.0).[154] Copyright 2020, The Authors, published by
American Association for the Advancement of Science.
circuit with a unique resonant frequency under zero pressure develop a flexible wireless pressure sensor based on the fabric
was formed by the integration of a pressure-sensitive capaci- spacer, which was sandwiched by two separate layers of pas-
tive element with an inductive antenna. Under an applied force, sive antennas and ferrite films.[159] Under an external load, an
the resonant frequency of the resonant circuit was changed inductance was changed by the mechanical compression of the
due to the variations in effective coupling capacitance.[157] Bao flexible spacer and the decrease of distance between the fer-
and co-workers developed a flexible and biodegradable wireless rite film and the antennas, which could be transduced to the
sensing platform based on fringe-field capacitor technology.[30] shift of the resonance frequency. The wireless detection of the
The fringe-field capacitors can be used for highly sensitive sensor resonance frequency depended on the near-field electro-
detection of close objects. Any change in capacitance resulted in magnetic communication between the external receiver and the
resonant frequency variations of the inductor–capacitor–resistor sensing antenna. A similar wireless strategy for a biodegrad-
(LCR) circuit, which was monitored wirelessly via inductive able pressure sensor was reported based on polycaprolactone
coupling. The trend of wireless sensing continued in 2021, with (PCL) and poly(d-lactide) (PDLA) biodegradable polymers.[160]
passive wireless motional sensing based on a co-capacitive vari- In the reported sensor, the inductor coil generated an induc-
ation strategy. In this regard, Zhang et al.[158] developed a meso- tive current by resonance with the external antenna, which also
functional flexible silk-based wool keratin (WK) e-skin with supplied power for the wireless sensor. In this system, capacity
passive wireless sensing capability. Capacitors, resistors, spiral variations were generated by pressure-induced distance changes
inductors, and spiral inductors were used to form LCR passive between the wireless pressure sensor’s capacitor plates.
wireless sensors with resonant circuits. The coil was printed on Chemomechanical, Acoustic, and Multimodal Sensing: High-
the flexible SF/WK hybrid substrate to fabricate an LCR sensor performance mechanical transduction strategies and other
circuit where an increase in pressure caused a decrease in res- novel transduction approaches in e-skins have been proposed
onance frequency and tunable sensitive detection of applied recently. The efficient incorporation of these strategies into
pressure. Another wireless sensing strategy was proposed to the biodegradable e-skins is still in its infancy and the number
of reports is limited. Owing to their high efficiency and mul- single stimuli (e.g., vibration, pressure, and tensile strain) and
timodal characteristics, they can be integrated into the future a combination of multiple stimuli.
biodegradable sensing platforms to fabricate the next gen-
eration of biodegradable e-skins. In 2019, Wang et al.[161] intro-
duced a tactile sensor based on a chemomechanical transduc- 3. Biodegradable E-Skins: Design, Fabrication, and
tion strategy to accurately perceive the biological and chemical
Integration
signals for a sensor with high sensitivity and portability. They
achieved chemomechanical transduction using an elastic The “electronic revolution” and the emergence of ubiquitous
pyramidal array. The tactile sensors transduced the signals of electronics are cornerstones of modern advanced societies. Nev-
the biomarker-induced gas-producing reactions into electrical ertheless, serious challenges exist, such as the management
signals. This tactile sensor was portable and could be used of e-wastes and their environmental impacts. The leaching of
to quantify various target molecules, including interferon-γ, toxic chemicals (e.g., Cr, Pb, and Hg) used in semiconductor
adenosine, and carcinoembryonic antigen. This tactile chemo- electronics and the release of volatile compounds related to
mechanical transduction strategy enabled the perception of the incineration of plastics into the environment pose severe
bio/chemical signals for tactile sensors. The authors claimed hazards to human health and the environment. There are limita-
using this strategy, electrical signals were enhanced more than tions and concerns regarding the production, management, and
tenfold compared with traditional electrical biosensors. recycling of e-wastes, including the toxicity of the components,
Sensitive detection of voice and acoustic signals using piezo- a lack of sustainable processing methods, and the large amount
capacitive,[162] piezoelectric,[163] piezoresistive,[164] and triboelec- of energy consumed during the fabrication of solid-state elec-
tric[165] sensing platforms have been widely studied. However, tronics. To solve these shortcomings, next-generation electronic
previously reported skin-attachable sensing platforms could not devices based on renewable, biocompatible, and biodegradable
maintain uniform and linear sensitivity due to damping effects materials that programmably degrade to nontoxic byproducts
and mechanical resonance. In this regard, a vibration-respon- have attracted considerable attention (Figure 8). Such “green”
sive sensing strategy was introduced by Li et al. to remedy electronic materials are produced from low-cost natural mate-
these limitations.[8] The authors developed a conformable, rials using low-energy approaches. Under European Standard
ultrathin (<5 µm), and vibration-responsive e-skin based on regulation EN13432, at least 90% of green electronics-incorpo-
the transduction of the human voice into an electrical voltage rated materials must be converted into nontoxic components
with a flat frequency response and high/linear sensitivity of (e.g., biomass, CO2, and H2O) under the influence of fungi and
5.5 V Pa−1. The reported device was composed of Au top and other natural microorganisms within 6 months of abandon-
bottom electrodes, which could be used to precisely quan- ment.[166,167] The application of degradable materials in elec-
tify human voices based on neck skin vibrations. This e-skin tronics adds other niche advantages related to data privacy and
consisted of a diaphragm array, where the diaphragms were patient confidentiality. The programmable and natural degrada-
connected in parallel to accumulate the electric charges from tion of green electronics ensures permanent self-destruction,
capacitors and to increase the output signal. By attachment of thereby providing personal data privacy. Therefore, the applica-
the e-skin to the neck, it was vibrated by voice, which led to the tion of biocompatible and biodegradable electronic materials in
dynamic displacement of diaphragms and capacitance varia- wearable electronics such as e-skins can be advantageous and
tion between top and bottom electrodes. This device was there- alleviate adverse human influences on the environment.
fore promising for the development of next-generation voice-
recognition e-skins for various IoT and HMI applications.
Most sensing platforms operate under a single transduc- 3.1. Biodegradable Substrates
tion mechanism; thus, they can only detect and distinguish a
single stimulus. However, multimodal e-skins with the ability 3.1.1. Natural-Biopolymer-Based E-Skins
to detect multiple stimuli offer unique advantages for material
discrimination and texture recognition compared with con- Various natural materials, including animal-based materials
ventual e-skins. Therefore, achieving total tactile perception by (e.g., fish bladders,[131,184] chicken feathers,[132] and prawn
simultaneous sensing of strain, pressure, and vibration using shells[185]) and plant-based materials (e.g., tree flowers, stumps,
hybrid multiple transduction mechanisms is essential for the leaves, pollen, and roots[28]) have been used to fabricate flexible
fabrication of high-performance e-skin with capabilities that substrates and e-skins (Figure 9). The unique hierarchical 3D
exceed the human’s tactile perception. Recently, Lee et al.[5] structures, high porosity, presence of micro/nanostructures,
developed a stretchable multimodal device that operates on surface protuberances, elasticity, and mechanical robustness
the basis of the various electrical characteristics of piezoelec- of these materials have inspired the fabrication of active bio-
tricity, piezoresistivity, and triboelectricity. The device provided mimetic substances and plant-based e-skins.[186] The structural
material discrimination and texture recognition in a biomi- hierarchies in plant-based components provide high surface
metic prosthesis applied to a robotic hand. The authors fabri- contact, optimum thermal/electrical distribution, and active
cated the e-skin from a wrinkle-patterned silicone elastomer, a surface sites for the adsorption of various functionalities. In
ZnO NW/AgNW hybrid nanomaterial, and a thin elastomeric addition, the existence of surface micro/nanostructures and
dielectric layer with high surface roughness to mimic human protuberances strongly influences the stability, elasticity, and
fingerprints. The device exceeded the human tactile perception flexibility of plant-based sensors, which in turn enhances
capabilities and could be used to identify and distinguish both their sensing characteristics because of the improved surface
Figure 8. Development timeline of biodegradable sensors and e-skins (2008–2022). Image for “Implantable photonic crystal”: Reproduced with permis-
sion.[168] Copyright 2008, Springer Nature. Image for “Electro-active paper”: Reproduced with permission.[169] Copyright 2009, SPIE. Image for “Chemical vapor
sensor”: Reproduced with permission.[170] Copyright 2010, Elsevier B.V. Image for “Humidity & temperature sensor”: Reproduced with permission.[171] Copyright
2011, Elsevier B.V. Image for “Wireless sensors”: Reproduced with permission.[172] Copyright 2012, IEEE. Reprinted, with permission, from IEEE 25th Int. Conf.
on Micro Electro Mechanical Systems (MEMS), 2012, pp. 468–471. Image for “RF pressure sensor”: Reproduced with permission.[173] Copyright 2013, IEEE. Image
for “Transient hydration sensor”: Reproduced with permission.[174] Copyright 2014, Wiley-VCH. Image for “Cardiovascular sensor”: Reproduced with permis-
sion.[175] Copyright 2015, Wiley-VCH. Image for “PGS e-skin”: Reproduced with permission.[176] Copyright 2015, IEEE. Reprinted, with permission, from 2015
IEEE Sensors, 2015, https://doi.org/10.1109/ICSENS.2015.7370669. Image for “Touch e-skin”: Reproduced with permission.[177] Copyright 2016, Royal Society of
Chemistry. Image for “Eraser-based e-skin”: Reproduced with permission.[178] Copyright 2017, IOP Publishing. Image for “Skin-inspired e-skin”: Reproduced
with permission.[179] Copyright 2018, Elsevier B.V. Image for “Edible e-skin”: Reproduced with permission.[180] Copyright 2018, American Chemical Society.
Image for “Silk-based e-skin”: Reproduced with permission.[110] Copyright 2019, Wiley-VCH. Image for “Biocompatible woven e-skin”: Reproduced with per-
mission.[181] Copyright 2020, Wiley-VCH. Image for “Spider-web inspired e-skin”: Reproduced under the terms of the CC-BY Creative Commons Attribution 4.0
International license (https://creativecommons.org/licenses/by/4.0).[182] Copyright 2021, The Authors, published by Wiley-VCH. Image for “Ferroelectric edible
e-skin”: Reproduced under the terms of the CC-BY Creative Commons Attribution 4.0 International license (https://creativecommons.org/licenses/by/4.0).[100]
Copyright 2021, The Authors, published by Wiley-VCH. Image for “Self-powered e-skin”: Reproduced with permission.[183] Copyright 2022, Wiley-VCH.
contact. In addition, other characteristics of plant-based sen- tional capabilities, hollow-sphere architectures, high natural
sors, including their structural color, antibacterial response, abundance, uniform morphology, and ornamented hierarchical
superhydrophobicity/superhydrophilicity, antireflection proper- structure. These characteristics provide a strong potential for
ties, selective filtration potential, and adhesion characteristics, forming interlocked microstructures, which can be used for
can be feasibility tuned via the incorporation and modification the amplification and transfer of tactile stimuli to electrome-
of surface micro/nanostructures.[187,188] chanical receptors.[194] Also, the petal surface properties can
Pollen microcapsules are ideal candidates for the develop- be replicated to fabricate high-performance e-skins because of
ment of flexible e-skin devices because of their elasticity, func- the similarity between a petal’s surface micropapillae and the
Figure 9. Structural characteristics of a plant. Pollen (scale bar: 10 µm); petal (scale bar: 20 µm); leaf (scale bar: 25 µm); stem, (scale bar: 200 µm); root
(scale bar: 50 µm). Image for “Pollen”: Reproduced with permission.[189] Copyright 2012, Academic Journals. Image for “Petal”: Reproduced under the
terms of the CC-BY Creative Commons Attribution 4.0 International license (https://creativecommons.org./licenses/by/4.0).[190] Copyright 2015, Polish
Botanical Society. Image for “Leaf”: Reproduced under the terms of the CC-BY Creative Commons Attribution 4.0 International license (https://crea-
tivecommons.org./licenses/by/4.0.[191] Copyright 2014, PLOS. Image for “Stem”: Reproduced with permission.[192] Copyright 2015, Brazilian Society of
Floriculture and Ornamental Plants. Image for “Root”: Reproduced with permission.[193] Copyright 2011, Wiley-VCH. Flower pollen and petals sketched
and redesigned based on a model from www.clipstudio.net.
epidermal and dermal characteristics of human skin.[195] Fur- and a high degree of adhesion. Inspired by the structure of
thermore, dried petals exhibit a uniform mastoid-like micro- plant roots, by which a plant can stand firmly on the ground
structure array and few layers of hollow structures, which can via stretching of its fractal roots underneath, researchers intro-
enhance the pressure sensitivity of e-skins.[28,196] duced an interlocking layer by growing biomimetic roots under
Other parts of a plant (e.g., leaves, spines, and roots) can also the electrode to increase adhesion and to fabricate films with
be used for developing e-skins and various sensors. Recently, high stretchability.[199] These properties can address the adhe-
Cho and co-workers[197] developed a sweat-collecting patch for sion limitations resulting from differences in the intrinsic
continuous sweat monitoring; their patch was based on the for- physical and chemical properties between metals and polymers.
mation of cactus-spine-inspired wedge-shaped wettability-pat- Natural biopolymers, including chitosan, cellulose, starch,
terned channels on a hierarchical surface. The unique geom- alginate, fibroin, dextran, collagen, HA, and poly(glutamic acid),
etry of the channels and superhydrophobic/superhydrophilic can be used as biodegradable polymers for the fabrication of
effects facilitated sweat transport via the induced unidirectional e-skins.[200,201] Among natural flexible materials, cellulose is a
Laplace pressure, even in the vertical direction. well-known natural biopolymer, and cellulose-based membranes
Because of their well-ordered hierarchical/quasifractal struc- have been widely studied as promising candidates because of
tures and mechanical robustness, plant leaves can be excel- their unique combination of characteristics, which include bio-
lent candidates for biotemplates for the fabrication of 3D flex- degradability, renewability, dielectric behavior, piezoelectricity,
ible substrates.[186,198] Similarly, because of their exceptional low cost, high abundance, and good biocompatibility.[202–204]
mechanical properties, plant roots can be used at interfaces Because of these advantageous properties, cellulose has been
between electrodes and soft substrates to achieve stretchability used as a dielectric layer, substrate, gel electrolyte, binder, and
carbon-based material to fabricate flexible and wearable elec- and high compression (95% strain without fracture). This ionic
tronics.[205–208] Liang et al.[209] developed a highly porous paper gel can be directly adhered to human skin without inducing
with tunable conductivity from cellulosic fibers and carbon residual or harmful inflammatory responses. Lim et al.[211]
black, which could be used in the biodegradable e-skins. The described an approach for the fabrication of transparent and
developed cellulosic composite paper exhibited stable piezoresis- stretchable cellulose-based films. Their prepared films exhibited
tive responses over a wide range of pressures (1–5.5 MPa) for high transparency and flexibility and reached a maximum of
800 cycles. A composite paper with 7.5 wt% carbon black showed 233% elongation at the breaking point.
sensitivities of −0.514 (1–50 kPa) and −0.215 kPa−1 (1–250 kPa). Gelatin-based gels are unique biopolymers that enable the
This cellulose-based paper with embossed patterns provided sen- preparation of various water-soluble additives with no need for
sitive skin-like sensing and enabled the detection of penetrating harsh synthetic approaches and are environmentally friendly,
damage. Shao et al.[210] fabricated reinforced ionic gels with high exhibiting a high degradation rate. Gelatin-based materials have
mechanical strength, self-adhesion, and self-healing properties. been used in a wide range of applications, including tissue engi-
The ionic gel was synthesized by forming, in a polymer network, neering,[212] drug delivery,[213] and microrobotics.[214] However,
coordination bonds among metal ions, poly(acrylic acid) chains, these gels suffer from poor performance, limited stretchability,
and tannic acid-coated cellulose nanocrystals (TA@CNCs). TA@ stiffening, limited stability after staining, and a tendency to dry at
CNC acted as a dynamically connected bridge that imparted a ambient temperature. Baumgartner et al.[33] developed a specific
hierarchically porous network to the ionic gels, which provided resilient and biodegradable gelatin-based biogel for applications
remarkable mechanical characteristics, including high tough- in soft robots and electronics (Figure 10a). Despite being degra-
ness (5.60 MJ m−3), ultrastretchability (fracture strain of 2952%), dable in wastewater through enzymatic cleavage by wastewater
Figure 10. Natural biopolymer-based e-skin platforms. a) Resilient and entirely biodegradable gelatine-based biogels. Reproduced under the terms of
the CC-BY Creative Commons Attribution 4.0 International license (https://creativecommons.org/licenses/by/4.0).[33] Copyright 2020, The Authors,
published by Springer Nature. b) Transparent, flexible, and pressure-sensitive electroluminescent skin and high-resolution pressure distribution
imaging. Reproduced under the terms of the CC-BY Creative Commons Attribution 4.0 International license (https://creativecommons.org/licenses/
by/4.0).[37] Copyright 2020, The Authors, published by Springer Nature.
bacteria within 5 days, the prepared gel maintained its mechan- 3.1.2. Synthetic Polymer-Based E-Skins
ical characteristics for more than 1 year, providing 330 000 cycles
of operation for soft actuators. These biogels were prepared from Different synthetic polymers have been used in biomedical
naturally derived materials such as Zn and cellulose. Cellulose applications such as implants,[216] drug delivery agents,[217,218]
acted as a textile exoskeleton for soft pneumatic biogel actua- and separation methods.[219–221] They have also been identified
tors, and the incorporation of a biogel with Zn electrodes led to as potential candidates for the fabrication of film substrates for
an entirely degradable sensor skin. In another study, Jo et al.[215] green electronics applications.[222] For instance, PDMS, which
developed a stretchable, conformal, and water-permeable e-skin was approved by the National Heart, Lung, and Blood Institute,
using a silk protein hydrogel and a metallic nanowire network. exhibited excellent flexibility, stretchability, and biocompatibility
The silk protein hydrogels provided stability and stretchability for use in the development of e-skins.[223–225] Other biodegrad-
under hydration through the inclusion of Ca2+ ions and glycerol. able synthetic polymers, including poly(4-hydroxybutyrate),
The NW electrodes provided stability against severe hydration PCL, poly(3-hydroxyoctanoate), poly(l-lactide-co-ε-caprolactone),
and deformation. In addition, the reported hydrogel offered water poly(glycolic acid), poly(l-lactide), poly(1,8-octanediol-cocitrate),
and related biomolecules to the electrodes, which facilitated com- POMaC, poly(3-hydroxybutyrate) (PHB), PLLA, poly(dl-lactic
munication between the electrodes and the environment. acid) (PDLLA), poly(glycolide-co-caprolactone), and PGS,
To overcome the limited pixel density, low sensitivity, and low have been used in biomedical applications.[226] Boutry and co-
conformability in pressure-distribution-imaging approaches workers[29] prepared stretchable and biodegradable organic
in e-skins, Lee and co-workers[37] developed a flexible and materials for applications in biomechanical sensors based on
transparent electroluminescent skin, based on biodegradable two biodegradable elastomers: PGS and POMaC (Figure 11a). In
cellulose-based compounds which they used to provide real- cells and tissue, POMaC exhibited biocompatibility comparable
time high-resolution images related to the pressure distribution to that of the PLLA control, and the FDA has approved PGS
(Figure 10b). This electroluminescent skin was prepared from for biomedical applications.[227,228] Their degradation process
a transparent pressure-sensing water-based nanocellulose/tel- can be tuned by varying the polymerization conditions.[229] The
lurium–PEDOT:PSS nanowire nanohybrid network. The e-skin electrodes were fabricated by evaporating Mg on top of a bio-
showed a sensitivity greater than 5000 kPa−1 and a response degradable polymer substrate (PLLA). The biodegradable metal
time shorter than 1 ms. The two ultrathin films could be used Mg was used because of its biocompatibility, ease of processing,
to transduce spatial pressure into a conductivity distribution, and rapid hydrolysis rate.[230] Biodegradable mechanical yet
which provided a high-resolution (>1000 dpi) pressure image. stretchable skin-like materials (i.e., poly(sebacoyl diglyceride)-
The photonic skin was used to directly visualize different physi- graft-2-ureido-4[1H]-pyrimidinone unit (UPy) (PSeD-U) elas-
comechanical stimuli with eye-readable colorations via the close tomers) were prepared by designing a unique physical and
lamination of target substrates. covalent hybrid crosslinking structure based on the so-called
Figure 11. Synthetic-polymer-based e-skin platforms. a) Stretchable and biodegradable pressure and strain sensor. Reproduced with permission.[29]
Copyright 2018, Springer Nature. b) Schematic of the structure and performance of PSeD-U elastomers. Reproduced under the terms of the CC-BY
Creative Commons Attribution 4.0 International license (https://creativecommons.org/licenses/by/4.0).[231] Copyright 2020, The Authors, published
by Springer Nature.
sacrificial bonds reported by Chen et al. (Figure 11b).[231] The In this case, the biocompatibility and biodegradability of the
PSeD-U hydrogen-bond-crosslinked bioelastomers were pre- doping process also need careful consideration. Specific conju-
pared via the incorporation of physical hydrogen bonds and gated polymers including PANI, polypyrrole (PPy), and PEDOT
covalent crosslinks to generate hybrid crosslinked networks. with conductivities up to 4.6 × 103 S cm−1 have been introduced
PSeD-U exhibited various advantages, including ease of fabrica- as degradable conductive polymers.[233] Mechanical limitations
tion, facile functionalization, good elasticity, good self-healing including brittle structure and stiffness in conjugated polymers
ability, biocompatibility, cytocompatibility, and biodegradability, can be remedied since high electrical conductance is achievable
which were defined as the refined version of PGS.[231] Upon at a low concentration of conjugated polymer within a specific
optimization of the hydrogen bonds in the elastomers, the composite.[234] Blending conjugated polymer nanoparticles with
toughness and strength were enhanced 11-fold and threefold, biodegradable insulating polymers is one strategy to prepare
respectively, compared with those of the covalent crosslinked the biodegradable conducting polymers, which exhibit type I
PSeD elastomers. An entirely biodegradable pressure sensor degradation. Furthermore, adjustment of polymer nanoparticle
for arterial blood flow measurements in both contact and concentration is essential for reaching the optimum values of
noncontact modes was fabricated.[30] Because of its biodegra- electrical conductivity. For example, a conductive composite of
dability, a secondary pressure for implant removal was unnec- HA doped PEDOT nanoparticles (PEDOT-HA) within PLLA,
essary. POMaC, PHV, PHB, PLLA, and PGS polymers were with conductivities as high as 4.7 × 10−3 S cm−1 was obtained
used to produce this pressure sensor. The implanted sensor by 10% nanoparticle loading. The presence of PEDOT-HA
was harvested after 12 weeks and exhibited partial degradation, accelerated the degradation process of PLLA by 10% after 8
where all the sensor components, including the PGS microp- weeks.[235] Furthermore, PEDOT-HA/PLLA did not exhibit a
yramids, POMaC sealing layer, Mg wires, and PLLA thin film, significant cytotoxic effect on PC12 cells during the degradation
were degraded; only PHB/PHV remained, consistent with the process. Contrary to type I polymers, type II polymers do not
reported rates of degradation for these materials. A biodegrad- show high electrical conductivities. Therefore, they generally
able composite of PLGA and PCL was developed by Khalid have been used to provide the stimulating small bioelectrical
et al.[232] and used for the fabrication of a piezocapacitive pres- signals in electronic platforms. By tuning and controlling the
sure sensor. The authors prepared a PLGA–PCL composite structural characteristics and doping properties, the conduct-
nanofiber membrane by electrospinning and subsequently used ance gap between type I and type II can be reduced. Rivers
it as an elastic dielectric membrane in a biodegradable sensor. et al.[236] prepared a biodegradable, electrically conducting
The results showed that this composite degraded in a phos- polymer composed of pyrrole-thiophene-pyrrole trimers and
phate-buffered saline solution and lost approximately 60% of aliphatic chains linked with ester bonds. Using iodine doping,
its initial weight in 2 weeks, with minimal loss of sensing per- the reported polymer exhibited an electrical conductivity of
formance after 1 week of incubation. In addition, the reported 10−4 S cm−1. In addition, after 2 weeks in PBS at body tempera-
device degraded further until 18 days. ture (37 °C) the degradation products were detected in the pres-
ence of the enzyme esterase. The toxicity study of degradation
products exhibited the nontoxicity of films and their degrada-
3.2. Biodegradable Active Layer tion products, and cytotoxicity of the iodine dopant. The non-
iodine strategy was proposed by Guimard et al.[237] to develop
Fabrication of biodegradable active layer is another pivotal chal- biodegradable and biocompatible conducting polymers, using
lenge in the development of biodegradable e-skins, sensors, a novel copolymer, 5,5′′′-bis(hydroxymethyl)-3,3′′′-dimethyl-
HMIs, and robotics platforms. Generally, a typical biodegrad- 2,2′:5′,2′′:5′′,2′′′-quaterthiophene-co-adipic acid polyester
able material consists of an active layer including a dielectric (QAPE), which consists the biodegradable ester units. The
layer, conductors, and semiconductors that are dispersed in a authors confirmed the biodegradation of the reported polymer
biodegradable matrix.[201] The conjugated polymers are used in by detection of a fluorescence signal, at wavelengths related to
conductors and semiconductors as active materials to provide the quaterthiophene subunit for degradation samples.
the electron conduction pathways within the specific matrix, Achieving higher electrical conductivity (>10−1 S cm−1) for
whereas dielectric materials benefit from high dielectric constant biodegradable conductors is limited to the corrodible Mg and
fillers and components as active materials. The biodegradable Fe electrodes, although the mechanical limitations including
materials can be classified into two major categories including stretchability, flexibility, and robustness hindered the wide-
type I polymers with disintegration without full chemical break- spread application of these materials as biodegradable con-
down, as well as type II, which can be recycled into oligomeric ductors. Therefore, the fabrication of elastic and stretchable
and monomeric building blocks. Because of the full biodegra- materials with high electrical conductivity will significantly
dability of type II materials, they can potentially be recycled.[201] contribute to the field of biodegradable, stretchable, and flexible
Therefore, understanding the chemistry, characterization, and electronics.
biodegradation mechanisms related to each category is essential. Fabrication of novel biodegradable semiconducting mate-
rials that offer ambient stability, high performance, and
solution processability is critical in the development of wear-
3.2.1. Biodegradable Conductors and Semiconductors able electronics. Well-known semiconducting polymers are
polythiophenes (e.g., poly(3-hexylthiophene) (P3HT))[238]
Various conductive conjugated polymers have been used as and donor-acceptor copolymers (e.g., diketopyrrolopyrroles
interconnects and conductive contacts by doping strategy. (DPP), (E)-2-(2-(thiophen-2-yl)vinyl)thiophene,).[239,240] Due
to the limitations related to conjugated structure, most of the constant (κ) such as metal oxides including SiO2, Al2O3, and
fabrication strategies discussed above for the preparation of hafnium oxide (HfO2) into a degradable polymer matrix.
conducting biodegradable polymers apply to semiconducting Deshmukh et al.[251] prepared the biopolymer nanocomposites
polymers. The blending strategy was used in presence of con- of cellulose acetate (CA) and Al2O3 nanoparticles. By the addi-
duction polymer to fabricate semiconductor polymers with tion of 25 wt% Al2O3 loadings, the dielectric constant increased
type I degradation. In addition, specific polymers including from 8.63 (50 Hz, 30 °C) for the neat CA matrix to 27.57 (50 Hz,
the P3HT and poly(3-thiophene methyl acetate) (P3TMA), were 30 °C) for CA/Al2O3.
used for blending with thermoplastic polyurethane (TPU), The cellulose nanofiber (CNF), which is a biodegradable
poly(tetramethylene succinate), poly(ester urea), and PLA to material derived from wood has attracted considerable atten-
increase the miscibility. Another challenge in the fabrication of tion because of its unique characteristics including low coeffi-
semiconductor polymers is attributed to the stiffness and rigid cient of mechanical robustness (200−400 MPa), thermal expan-
characteristics of semiconducting molecules. Furthermore, the sion (12−28.5 ppm K−1), Young’s modulus (7.4−14 GPa), and
presence of charge-transporting aggregates is another limita- great potential for replacement of nondegradable polymers.[252]
tion of the widespread use of semiconducting polymers in flex- In this case, Zeng et al.[253] developed flexible dielectric papers
ible and stretchable wearables. In this regard, Fabiano et al.[241] based on CNTs and biodegradable CNFs for dielectric energy
proposed the confinement of semiconducting polymers into storage applications. The reported paper exhibited a high dielec-
weakly ordered fibers within an inert polymer matrix without tric constant of 3198 at 1.0 kHz and enhanced dielectric energy
affecting their charge transport properties. In this system, the storage capability of 0.81 ± 0.1 J cm−3, which was attributed to
semiconducting polymer chains were prevented from attaining the low content of CNTs (4.5 wt%). Mechanically, the CNF/CNT
long-range order, yet remained extended along the backbone papers exhibited good flexibility, while the tensile strength and
direction and aggregate. As a result of this confinement, the Young’s modulus reached 116.7 ± 13 MPa and 8.2 ± 0.7 GPa,
obtained polymer films kept the high mobility even at very low presenting an increase of 22.8% and 36.7%, respectively, com-
concentrations. pared with those prepared from pure CNF paper. Other biode-
To develop the type II biodegradable semiconductor poly- gradable candidates including banana, bamboo fibers, and jute,
mers, Lei et al.[242] fabricated totally disintegrable flexible cir- have also been incorporated into dielectric composite materials,
cuits and a fully biocompatible and decomposable semicon- with enhanced dielectric constant.[254] Dielectrics also may be
ducting polymer. Harnessing the reversible imine chemistry, a chosen among nucleobases including guanine and adenine,
fully decomposable conjugated polymer with high charge car- as well as various sugars such as glucose, sucrose, lactose, or
rier mobility was prepared, which was comparable to traditional even caffeine. Glucose, adenine, and guanine are excellent
conjugated polymers in electrical performance solution pro- dielectrics, with high breakdown strengths and low dielectric
cessability. Also, the authors prepared a thermally and chemi- losses.[255] Other than natural biodegradable dielectrics, syn-
cally stable ultrathin cellulose film for application in transient thetic biodegradable polymers such as PGS also exhibited inter-
and biodegradable electronics. esting dialect properties. Boutry et al.[175] developed a fully bio-
Other suitable semiconducting materials are melanins, degradable and biocompatible pressure sensor based on PGS
which are natural conductive pigments with unique physical dielectric layer with rapid response, high sensitivity, and good
and electrical characteristics.[243] The electrical conductivity of dielectric properties.
melanins depends on the physical form, the hydration state,
and temperature, ranging from order of 10−8 S cm−1 in the
dehydrated state to 10−3 S cm−1 in the fully hydrated state.[244] 3.3. Biodegradation Mechanism
Langer and co-workers[245] prepared melanin films with conduc-
tivities of 7.00 ± 1.10 × 10−5 S cm−1 in the hydrated state. In addi- In general, two routes of hydrolysis and oxidation were proposed
tion, semiconducting melanin implants were biocompatible, for the degradation of biodegradable compounds.[201] Ester
biodegradable, and fully degraded after 8 weeks. bonds in the PLA, PGL, PCL, and polycaprolactone are suscep-
tible to hydrolytic degradation.[256] Other degradable moieties
such as imide, amide, urethane, thioester, carbonate, anhydride,
3.2.2. Biodegradable Dielectrics urea, and imine bonds degrade under chemically and enzy-
matically hydrolytic reactions. In addition, different parameters
In general, the polymer-based dielectric materials mainly affect the rate of hydrolyses such as temperature, the number of
include nonrenewable and nondegradable polymers including hydrolyzable functionalities, cross-linking density, crystallinity,
biaxially oriented polypropylene (BOPP),[246] polyvinylidene the chemical composition of the medium, and morphology.[257]
difluoride (PVDF),[247] thermosetting polymers, such as Complementary to hydrolysis degradation, oxidation is
polyimide,[248] epoxy,[249] and divinyltetramethyldisiloxane– another biodegradation route, which is induced by biologically
bis(benzocyclobutene) (BCB).[250] Therefore, efficient design and active elements that lead to chemical and enzymatical degra-
development of dielectrics with a renewable and biodegradable dation of polymers. Phagocytes are immune cells that protect
nature is essential. Different types of natural and synthetic bio- the body from bacteria, viruses, and dying cells by enrolling in
degradable materials are available for the development of die- an early and late immune response. Phagocytes play a critical
lectrics with engineered physical and electrical properties. One role in releasing free radicals, which contribute to the forma-
important approach for the fabrication of biodegradable dielec- tion of nitric oxide synthase (NOS) and reactive oxygen species
trics includes the incorporation of fillers with high dielectric (ROS) and the initiation of the polymer depolymerization by
Figure 12. Biodegradation mechanism. a) Fabrication and decomposition cycle of disintegrable polymer (PDPP-PD). Reproduced with permission.[242]
Copyright 2017, The Authors, published by National Academy of Sciences, USA. b) Design of fully degradable semiconducting polymer films through the
nanoconfinement effect, chemical structure of E-PCL, and biodegradation pathway of fully degradable semiconducting polymer, p(DPP-PPD). Repro-
duced with permission.[258] Copyright 2019, American Chemical Society (https://pubs.acs.org/doi/full/10.1021/acscentsci.9b00850); further permis-
sions for the material excerpted should be directed to the ACS.
oxidation.[257] Susceptible functionalities to oxidative cleavage rated PHA with thiol-ene click chemistry led to the production
include aldehydes, ethers, amines, alcohols, phenols, allylic of poly[(R)-3-hydroxybutyrate-co-(R)-3-hydroxy-10-undecenoate]
carbons, and aromatic cycles are all susceptible to oxidative (PHBU). The PHAs are groups of natural biodegradable and
cleavage.[257] biocompatible polyesters that are produced by a variety of
Lei et al.[242] proposed key steps of the “ideal cycle” in bio- microorganisms.[260,261] By cross-linking the PHBU polymer, a
degradation of polymers (Figure 12a) by fabrication of entirely 200% to 26.2 MPa tensile strength enhancement was observed,
disintegrable conjugated polymer. The authors reported a bio- without causing significant cytotoxicity toward human
degradable ultrathin (800 nm) substrate based on cellulose for cells.[260,261]
ultra-lightweight electronics (2 g m−2). In addition, this polymer Biodegradable encapsulation in e-skin was achieved using
reached complete disintegration (PDPP-PD) after 30 days. In biodegradable synthetic and natural encapsulants including
2019, a two-component fully degradable, polymeric system PLGA, chitosan, and cellulose-derived thin films. Recently, chi-
was reported,[258] which could be self-assembled into nano- tosan was used for the fabrication of TENG-based multifunc-
confined semiconducting fibril aggregates to provide stretch- tional e-skin with high transparency, sweat permeability, con-
ability (Figure 12b). In this system, both the semiconductor trollable biodegradability, and self-powered sensing capability
and matrix were entirely degraded into monomeric constituent based on ultrathin and stretchable transparent Au nanofiber
components. In addition, the authors used a well-established electrodes.[183] In this device, the thin chitosan membrane was
biodegradable urethane-based polymer featuring polycaprolac- used for biodegradable encapsulation of Au nanofiber elec-
tone (E-PCL) as an elastomeric matrix. trodes. The chitosan membrane was fabricated via a green solu-
tion-casting approach. Moreover, by the addition of glycerol, the
water vapor permeability, flexibility, and hydrophobicity of the
3.4. Biodegradable Encapsulation membrane were improved. Another biodegradable TENG was
developed as an implantable power source.[129] In this platform,
To ensure the stable performance of a device in dynamic con- the whole structure was encapsulated in PLGA and PVA layers.
ditions, various types of biodegradable elastic encapsulants At ≈50 days, the encapsulation layer of the device was hydro-
have been introduced to protect the air- and water-sensitive lyzed into a viscous gel of low-molecular-weight PLGA, which
components. The lack of desirable stretchability in well-known led to the loss of structural integrity of the platform. In 2020,
biocompatible materials such as cellulose, silk, PCL, and PLA Baumgartner et al.[33] developed fully degradable elastic gelatin-
has led to the development of other biodegradable elastomers based biogels for application in electronics and soft robotics.
including PGS, polyhydroxyalkanoates (PHAs), PCL-based ure- The authors described a fully biodegradable encapsulation by
thanes, and poly(1,8-octanediol-co-citrate).[174] In this regard, dip coating of G2430 biogel in shellac solution. The encapsula-
Langer and co-workers developed a tough, biodegradable, and tion layer was degraded in basic solutions, which was followed
flexible elastomer PGS fabricated from biocompatible mono- by the complete dissolution of fabricated biogels. The biore-
mers.[104] The PGS was implanted in rats and totally absorbed sorbable and biodegradable polyanhydride polymer was used
after 60 days. In addition, blending and cross-linking strategies for encapsulation of bioresorbable metal coils and substrates
can also enhance mechanical properties. Blending provides in implantable, multifunctional silicon sensors for the brain, in
the feasible modification of physical properties, such as glass which all constituent materials could be naturally resorbed via
transition temperature, melting temperature, crystallinity, and hydrolysis, eliminating the necessity for the extraction or addi-
mechanical characteristics. The blending of PGS with PCL tional surgical operation. In another research, the polybutylene
enhanced the extensibility, elastic modulus, and mechanical terephthalate (PBAT) biodegradable elastomeric substrates
robustness.[213,259,260] Furthermore, the cross-linking of unsatu- (100 µm thickness) were used as a biodegradable encapsulation
Figure 13. Structure and degradation of bioresorbable sensing platform. a) Schematic of passive bioresorbable neural electrode array for clinical
electrocorticography and subdermal encephalograms measurements (Reproduced with permission.[268] Copyright 2016, Springer Nature. b) Wireless-
powered full wave rectifying system with an Mg receiving antenna and RF transmitter. Reproduced with permission.[269] Copyright 2013, Wiley-VCH.
c) Structure of a biodegradable, capacitive, and stretchable EP sensor. Reproduced with permission.[270] Copyright 2015, American Chemical Society.
layer in fully biodegradable MgZnCa metallic glass (MG) film ings (Figure 13a). The authors described the fabrication of fully
for application in intrinsically stretchable electrodes.[262] bioresorbable electrode arrays. In this device, a film of and a
The PCL is another candidate that can be used in the biode- foil of PLGA (≈30 µm thick) and SiO2 (≈100 nm thick) served
gradable encapsulation of biodegradable magnesium/iron bat- as a bioresorbable substrate and an encapsulating layer. In
teries. The use of PCL encapsulation minimized the volume of another work, Rogers and co-workers[269] reported a bioresorb-
electrochemical cells and provided higher discharge rates and able material for RF applications, which is important in diverse
longer discharge lifetimes. A 5 µm-thick PCL layer was utilized electronic operations such as data transmission and power
as both battery packaging material and a permeable coating supply. The same research group described the involvement
suitable for the physiological solution to penetrate and activate of biocompatible and water-soluble constituent materials, that
the developed battery.[263,264] Moreover, the thin PCL coating is, magnesium (Mg; conductors), silicon nanomembranes (Si
enhanced the Coulombic efficiency and specific capacity of the NMs; semiconductors), silk (substrates), and silicon dioxide or
Mg/Fe electrochemical cells. Because PCL is an FDA-approved magnesium oxide (low-temperature SiO2 or MgO; interlayer
biodegradable polymer, PCL coatings can be utilized for the dielectrics), in the fabrication of transistors, antennas, capaci-
fabrication of Mg-based implantable biodegradable batteries tors, rectifying diodes, RF energy harvesting sub-systems, resis-
and transient implantable medical devices (TIMDs).[263,264] The tors, ring oscillators, and inductors (Figure 13b). In addition,
PLLA or PLA are other FDA-approved biodegradable polymers, they utilized a uniform layer of MgO (≈500 nm thickness) for
which have been used in implanted medical devices, tissue the encapsulation of diodes. Other biodegradable elastomers
engineering, and drug delivery.[14] For example, PLLA was used and silicon nanomembranes for transient and stretchable elec-
as biodegradable encapsulation layers for molybdenum wires in tronics were developed based on using Si nanoribbons and
nanofiber-based piezoelectric transducers.[14] nanomembranes on a biodegradable elastomer (poly(1,8-octane
E-skin and sensing platforms based on bioresorbable mate- diol-cocitrate)) to fabricate a stretchable platform with linear
rials have been reported for biomedical applications ranging elastic mechanical responses (Figure 13c).[270] The authors used
from drug delivery,[265] to stents[266] and sutures.[267] In this a uniform overcoat of plasma-enhanced chemical vapor deposi-
regard, various bioresorbable components of e-skin including tion SiO2 to encapsulate the entire system.
power supply, circuits, antenna, and electrodes have been devel- Efficient application of biodegradable e-skins in extreme
oped using biodegradable materials. Rogers and co-workers[268] environments such as high humidity and freezing ecosys-
developed bioresorbable silicon electronics for cerebral cortex tems is another critical challenge, which should be addressed
transient spatiotemporal mapping, which could detect epilep- properly because these circumstances can disturb the struc-
tiform and physiologic activity in chronic and acute record- ture and performance of e-skins in resource-limited settings.
In one research, Ke et al.[271] developed a degradable collagen- categories of durable materials are suitable candidates for
based humid-ultrastable e-skin based on the cowskin as a encapsulation of e-skin components for extreme environment
deformable 3D sensory substrate. The reported e-skin was applications.
superhydrophobic, with unaffected sensory performance
under extreme humidity (50 °C and relative humidity of
82%). In 2022, a gelatin-based zwitterionic organohydrogel 4. Recent Advances in Applications of
was introduced for long-term moisturizing and antifreezing
Biodegradable E-Skins
characteristics for application in e-skins and wearable elec-
tronics. Because of the dense cross-linked network of gelatin Biodegradable e-skin, which undergoes chemical and bio-
and zwitterionic organohydrogel, strong mechanical and logical breakdown into smaller fragments that are dissolved
strain properties were achieved. In addition, owing to the syn- or metabolized in their applied physiological environments,
ergistic interaction between zwitterionic groups and glycerol, has attracted considerable attention in biomedical science
the developed organohydrogel exhibited good antidehydra- (Table 3). The biodegradability enhances the applicability of
tion (over 7 days) and antifreeze resistance (−40 °C). These temporary medical implants and sensors for the real-time
Table 3. Summary of performance and applications of biodegradable nanogenerators, sensors, and e-skins.
Materials Mechanism Sensitivity & Performance Degradation Ref Application

Rose leaf and petal, AgNW Capacitive 0.08 kPa−1 75 days [28] Flexible tactile sensor, gesture
(0.007−60 kPa) monitoring, touch sensing
POMaC, PGS, PLLA, Magnesium Capacitive 0.70 ± 0.40 kPa−1 (p<1 kPa) 3.5 weeks [29] Pressure sensor for orthopaedic
0.13 ± 0.03 kPa−1 (5–10 kPa) application
Graphene, β-Glycine, Chitosan Piezoelectric 2.70 × 10−4 kPa−1 (5−20 kPa), – [51] Field-effect-transistor,
7.56 × 10−4 kPa−1 (20−35 kPa) large-area e-skins
PLGA and PCL Piezocapacitive 0.863 ± 0.025 kPa−1 (0 < P ≤ 1.86 kPa), 18 days [232] Pressure sensors, mapping of different
0.062 ± 0.005 kPa−1 (1.86 kPa < P ≤ 4.6 kPa) pressure points
Cellulose, MWCNT Piezoresistive −0.0197 kPa−1 (0−20 kPa) – [272] Flexible and pressure-responsive sensors,
smart clothing, medical diagnosis
AgNW, PLGA, PVA Triboelectric 0.011 kPa−1 AgNWs/PVA: [21] Real-time and self-powered monitoring of
3 days physiological signals and motions
AgNWs/PLGA:
21 days
PVA, Graphene, Acrylic ester, Ethanol, Piezoresistive GF: 502 DI water: 90 s, [35] HMI, strain sensor, physiological
Propylene glycol, Phenoxyethanol, Biological Skin: 8 h signal monitoring
Octoxynol-10, and Benzyl alcohol
PGS, MWCNTs, NaCl Piezoresistive 0.12 ± 0.03 kPa−1, 8.00 ± 0.20 kPa−1 8 weeks [16] Wearable devices, motion monitoring,
recreation, tissue engineering
Meso-poly(lactic acid) (meso-PLA), Triboelectric Output voltage: 70 V – [181] HMI, nanogenerator devices
PLLA Piezoelectric Current: 25 µA
Output power: 0.31 mW
Silk hydrogel, ZnO nanorods Triboelectric Output power: 1 mW cm−2 Enzyme/PBS: [273] HMI, biomedical implants,
Piezoelectric Energy harvest: 1h tactile sensors, soft robotics
Skin ≈6.2 µW cm−2
Tissues ≈0.9 µW cm−2
Silk fibroin, PAM, Graphene oxide, Triboelectric 0.0137 kPa−1 – [274] Wearable electronics, soft robotics,
PEDOT:PSS (0−15.9 kPa), 0.00238 kPa−1 health and exercise monitoring,
(15.9−119.4 kPa) and power sources
β-Glycine, Chitosan Piezoelectric 2.82 ± 0.2 mV kPa−1 48 h [77] Wearable biomedical diagnostics
Chitosan, β-Glycine Piezoelectric 1.42 mV (5–25 kPa) 24 h [275] Pressure Sensor, POC and implantable
diagnostics
Cellulose, Graphite Capacitive 0.003 kPa−1 2–3 weeks [276] Touch sensor
Chicken feather fiber Piezoelectric Output voltage: 10 V, Power density: 6 3 days stability [132] Energy harvesters, wearable electronics,
µW cm−2 Current density: 1.8 mA cm−2, bio-implantable and physiological
(0.13–0.31 MPa) monitoring platforms
Fish scale Piezoelectric Output voltage: 4 V, – [277] Self-powered Implantable diagnostics
Power density: 1.14 µW cm−2 devices and personalized medicine
Short circuit current: 1.5 µA
analysis and monitoring of various physiological parameters, In 2020, Elsayes et al.[28] reported a plant-based biodegradable
including pressure, temperature, strain, and oxygen, without capacitive tactile pressure sensor for the development of dispos-
the risk of post-surgery infections in the human body and able e-skins. Freeze-dried rose petals functioned as the dielec-
without the limitations imposed by toxicity, high costs, and tric layer, and decorated leaf skeletons functioned as breath-
corresponding environmental pollution. This section discusses able and flexible electrodes (Figure 14a). The leaf skeletons of
the recent developments in the fabrication and application of Ficus religiosa used in this study, which have a rough fractal-like
biodegradable e-skins in tactile sensors, robotics, and HMI architecture, facilitated the adhesion of AgNWs to provide inter-
platforms. connections between the AgNWs when the electrode was bent.
The rose-petal dielectric layer compressed elastically under
pressure, which was attributed to its multiscale 3D cell wall
4.1. Sensors microstructure. The reported biodegradable sensor exhibited a
sensitivity of 0.08 kPa−1 (0.007–60 kPa) and good signal stability
The selection of appropriate materials for the development for at least 5000 pressure cycles. The sensor was fully biode-
of biodegradable e-skin sensors is challenging because the gradable in tap water and phosphate-buffered saline solution
selected material should be biocompatible, conformal, non- (Table 3). Peng et al.[21] developed a biodegradable, flexible, and
toxic, and biodegradable, with enhanced mechanical, electrical, antibacterial all-nanofiber e-skin based on a TENG. The e-skin
and optical characteristics. Flexibility, stretchability, and spe- was prepared from PLGA, AgNWs, and PVA and could be used
cific mechanical properties for minimal stress and conformal for whole-body motion monitoring and physiological detection
interfacing with biological skin are other critical aspects of bio- (Figure 14b). Because of the biocidal characteristics of AgNWs,
degradable e-skins. The costs and abundance of renewable and this e-skin exhibited antibacterial behavior against Escherichia
biodegradable naturally derived materials, including animal- coli and Staphylococcus aureus. The service life of the reported
derived polymers (e.g., collagen, silk, and chitosan) and plant- e-skin could be tuned according to the selection and collocation
based polysaccharides (e.g., cellulose, alginate, and dextran), of biodegradable PLGA and PVA.
are important factors. In this regard, extensive studies have Another bioinspired flexible pressure sensor was reported
been conducted to select appropriate biodegradable materials based on a Ti3C2/natural microcapsule (Ti3C2/NMC) biocom-
for e-skin sensing applications.[274] For example, the field-effect posite film with robustness and deformability.[279] The film
transistor-based approach is a unique strategy for developing mimicked biological characteristics, such as interlocking, pat-
pressure sensors because of the high sensitivity, low signal- terning, and hierarchy. The reported films exhibited high
noise ratio, high spatial resolution, and active matrix recogni- deformability, with an elastic modulus of 0.73 MPa and a
tion capability of the resultant sensors.[278] In this regard, the sensing capability of 24.63 kPa−1, demonstrating a 9.4-fold
biodegradable piezoelectric GFET-based dynamic pressure increase in pressure sensitivity compared with a corresponding
sensor reported by Dahiya et al.[51] that could be fully degraded planar-structured Ti3C2-based flexible sensor (2.61 kPa−1), along
by replacing the Cu electrode in the piezoelectric transducer with a 14 ms response rate and good stability over 5000 cycles.
layer of the MIM assembly with a degradable metallic electrode The authors used natural sea-urchin-shaped microcapsules
material such as Mg. (Helianthus annuus L. spores) with hollow structures as the
Figure 14. Natural and synthetic biodegradable e-skin platforms. a) Structure of a plant-based capacitive tactile pressure sensor. Reproduced under
the terms of the CC-BY Creative Commons Attribution 4.0 International license (https://creativecommons.org/licenses/by/4.0).[28] Copyright 2020,
The Authors, published by Wiley-VCH. b) All-nanofiber TENG-based e-skins with stretchability, sensor performance, and biodegradability. Reproduced
with permission.[21] Copyright 2020, The Authors, published by American Association for the Advancement of Science. From ref. [21]. © The Authors,
some rights reserved; exclusive licensee AAAS. Distributed under a CC BY-NC 4.0 license http://creativecommons.org/licenses/by-nc/4.0/. Reprinted
with permission from AAAS.
Figure 15. Application of biodegradable and biocompatible e-skins in the HMI and robotics. a) Illustration of the MXene/tissue-paper-based sensors
and degradability in a NaOH solution. Reproduced with permission.[284] Copyright 2019, American Chemical Society. b) Fabrication, stretchability, self-
healing, and sensing of PBS hydrogels. Reproduced with permission.[285] Copyright 2019, American Chemical Society. c) Characteristics of the GNF
sensor. Reproduced with permission.[35] Copyright 2018, Wiley-VCH.
building blocks for the formation of interlocked structures. The biodegradable hybrid nanogenerator containing a piezoelectric
proposed structure provided efficient signal transduction and PLLA film and a meso-poly(lactic acid) (meso-PLA) electret-based
mechanical resilience. TENG. The authors combined the high current of a double-
In one study, Wang et al.[147] fabricated a combination tem- layered PLLA-based PENG and the high output voltage from a
perature–pressure e-skin based on silk-nanofiber-derived nonpiezoelectric meso-PLA electret-based TENG to develop an
carbon fiber membranes (SilkCFM). The reported sensor exhib- e-skin HMI device. The resultant nanogenerator produced a
ited high strain sensitivity (GF of ≈8350 at 50% strain) and current of 25 µA and an output voltage of 70 V at a resonance
good temperature sensitivity (0.81% per degree Celsius). The frequency of 19.7 Hz. The hybrid nanogenerator showed 11%
SilkCFM in each sensor was passive to other stimuli, enabling higher output power than the corresponding PLLA-based
the simultaneous detection of temperature and pressure by the PENG.
e-skins. Recently, Han et al.[280] designed an ionic-conductive The fabrication of e-skins with broad sensing capabilities
gluten based on glycerol and ions. Glycerol, ions, and the pep- (as high as 30 kPa), high sensitivity, long-term stability, rapid
tide chains in gluten exhibited strong interactions, which led response, low e-waste production, and biodegradability is a
to good conductivity, flexibility, and mechanical robustness critical challenge. In this case, Guo et al.[284] developed a flex-
(strength of 150 kPa and elongation of 600%). The gluten also ible wearable transient pressure sensor based on MXene for
showed biocompatibility and degradability (it degraded in 1 m sensitive, degradable, wireless, and broad-range HMIs. The
KOH within 6 h). The reported device exhibited good stability sensor was prepared by impregnating MXene nanosheets
for 3000 cycles and was used as skin strain sensor to detect into tissue papers and sandwiching between a biodegradable
both large-scale movements (e.g., finger, wrist, and elbow PLA sheet and an interdigitated electrode-coated PLA sheet
bending) and subtle motions (e.g., frown, swallow, and blow- (Figure 15a). The sensors demonstrated low power consump-
scale motions). tion (10−8 W), a low detection limit (10.2 Pa), high sensitivity, a
short response time (11 ms), biocompatibility, biodegradability,
and reproducibility for more than 10 000 cycles. The authors
4.2. Human–Machine Interfaces and Robotics reported that this sensor could be used to input Morse code by
touching the sensor surface, which can be connected to a wire-
The efficient conversion of natural human motions to elec- less transmitter for wireless HMI sensing. One biocompatible
trical signals, which can be used to control/charge electronic ionic hydrogel was developed based on PVA, SF, and borax.[285]
systems in HMI platforms, has been investigated extensively In this ionic hydrogel and related ternary system, borax and
for biomedical science, electronic engineering, and analytical PVA provided high conductivity and stretchability, respectively.
chemistry.[40,281–284] Gong et al.[181] developed a biocompatible, The SF stabilized the hydrogel and enhanced water uptake by
the gels (Figure 15b). The resultant hydrogel exhibited good 5.1. Design and Configuration
adhesion, high stretchability at strains greater than 5000%,
self-healing ability, and adjustable conductivity. Another biode- The bulky design and nonbiodegradable structure of traditional
gradable silk-based electronic tattoo (e-tattoo) for applications power supply adversely affect the efficient performance of
in HMI, artificial intelligent robotics, self-powered devices, e-skins. Therefore, a need exists to design and fabricate high-
and prosthesis was introduced in 2021.[286] This self-powered performance biodegradable self-powered or wireless-powered
platform offered a skin-compatible, ultra-thin, biocompatible, platforms. In one study, Jiang and co-workers[288] developed
and biodegradable characteristics based on a silk nanofiber/ fully bioabsorbable and biodegradable natural-materials-based
carbon nanotube/silk nanofiber (SNF/CNT/SNF) TENG device TENGs (BN-TENGs) using five natural components: cellulose,
with on-skin energy harvesting capabilities (power density of chitin, SF, rice paper, and egg white. The “triboelectric series”
≈6 mW m−2). In addition, the reported e-tattoo was slowly disin- of the reported components were ranked on the basis of their
tegrated and disappeared in PBS after 8 days, which confirmed abilities to gain or lose electrons from positive to negative as
the biodegradability of the platform. Wan et al.[35] developed follows: egg white > SF > chitin > cellulose > rice paper. This
a skin-conformal, stretchable, and biodegradable graphene- nanogenerator exhibited a maximum voltage, current, and
based sensor for HMI applications. The high adhesion (peel-off power density of 55 V, 0.6 µA, and 21.6 mW m−2, respectively.
strength of ≈29.4 N m−1) and ultraconformity to skin led to a The encapsulation by SF enabled the operation time of the
14.2-fold signal amplification (Figure 15c). The sensor exhibited nanogenerator to be tuned from days to weeks. In addition,
high sensitivity, rapid response, and a stretchability (≈35%) com- after completing its function, the reported nanogenerator was
parable to that of human skin (≈30%). In addition, the described fully degraded and resorbed in Sprague–Dawley rats, avoiding
sensor was biodegradable and degraded in DI water because it a secondary removal operation. Another biodegradable TENG
was prepared from a water-soluble polymer. In another study, a was developed based on a multilayer structure composed of bio-
biocompatible, biodegradable, and stretchable silk hydrogel was degradable polymers, including PLGA, poly(3-hydroxybutyric
developed as an artificial piezoelectric energy-generating skin acid-co-3-hydroxyvaleric acid) (PHB/V), PCL, PVA, and a resorb-
(EG-skin) to harvest the electrical energy from biomechanical able metal, such as Mg.[129] The reported polymers were low-
motion.[273] In this skin, ZnO nanorods incorporated into the cost, commercially available, soluble materials that tended to
silk hydrogel generated an eightfold increase in piezoelectricity gain or lose electrons. Also, the reported TENG was degraded
compared with the pristine silk hydrogel, a twofold enhance- and resorbed in an animal body after completing its work cycle.
ment in the electrical response, and power generation of The open-circuit voltage of biodegradable TENG reached ≈40 V
1 mW cm−2. Because of its softness, stretchability, and skin- with a short-circuit current of ≈1 mA. He et al.[289] reported
adhesive properties, the EG-skin conformally interfaced with a self-powered antibacterial cellulose fiber-based TENG (cf-
tissues and biological skins and generated an output power of TENG) system based on environmentally friendly cellulose
0.9 and 6.2 µW cm−2 from their motions and physical activities, microfibers/nanofibers and Ag nanofibers. The reported cf-
respectively. A cellulose-derived TENG was designed[287] on the TENG demonstrated PM2.5 removal capability (efficiency of
basis of the tribopolarities between crepe cellulose paper (CCP) 98.83%), which is a fine particulate matter (≤2.5 µm) respon-
and a nitrocellulose membrane (NCM), and their microstruc- sible for various allergy types and the spread of respiratory dis-
tures. This CCP/NCM paper-based triboelectric nanogenerator eases. With this system, the breathing rate and intensity could
(P-TENG) demonstrated triboelectric behavior and a power den- be detected because of the electricity production dependence of
sity of 16.1 W m−2 over 10 000 cycles. The reported P-TENGs cf-TENG on various operating displacements and frequencies.
demonstrated mechanical energy harvesting capability, self-
powered sensing, and HMI characteristics. In addition, the
P-TENGs were fabricated from biodegradable, abundant, low- 5.2. Powering and Energy
cost, and renewable cellulose (CCP and NCM).
The wireless powering of electronics and detection units in
e-skins and sensors is another challenge that has attracted
5. Main Challenges in Applications extensive attention in recent years. One important powering
strategy is attributed to the application of self-powered TENG-
of Biodegradable E-Skins
based devices, which were discussed comprehensively in pre-
Despite the significant advances in fabrication approaches and vious sections. However, there are some other strategies for
applications of biodegradable e-skins in sensing, HMIs, inte- powering biodegradable e-skins such as wireless powering and
grated electronics, and biomedical engineering, further inno- biocatalyst-based approaches. Guo and co-workers[290] described
vations and improvements are needed to achieve performance a strategy for the wireless supply of power to biodegradable
comparable to that of their nondegradable counterparts. More- electronics using a specific bioresorbable system in which a
over, there are serious challenges regarding commercialization, rotating permanent magnet acts as a transmitter and a biore-
standardization, clinical approval, and applications of biode- sorbable antenna serves as a remote receiver for operation at
gradable e-skins in healthcare facilities. Several limitations frequencies lower than 200 Hz. This system can be used as
hamper the approved use of biodegradable e-skins for real-life an additional alternative for providing wireless power to tem-
biomedical applications, including insufficient mechanical porary implants. Other strategies for providing stable and sus-
resilience, low conductivity, and poor stretchability in plant- tainable power sources for the steady operation of e-skins have
based electronic devices and biodegradable power supplies. been reported. For instance, Mohammadifar et al.[39] described
an innovative strategy for providing long-term energy via the as water diffused into the bulk-degrading polymer substrates,
metabolisms of sweat-eating bacteria that exist on human skin: although the diffusion of water could be hindered by encap-
Micrococcus luteus, Staphylococcus capitis, and Staphylococcus epi- sulation. The authors claimed that the application of bioac-
dermidis. Sweat-powered batteries based on microbial fuel cells tive glasses improved the stability of bioresorbable sensors. In
(MFCs) were prepared using skin-inhabiting sweat-eating or addition, this resonance sensor operated at distances sufficient
non-human ammonia-oxidizing bacteria, which acted as a bio- for applications beneath the skin. However, longer reading dis-
catalyst to convert the chemical energy of sweat into electrical tances might be achieved using bioresorbable materials with
energy. The authors reported that specific types of microorgan- higher electrical conductivities or thicker conductors. A battery-
isms can transfer extracellular electrons from sweat and func- free and perspiration-powered e-skin for the in situ sensing
tion as a biocatalyst in an MFC, which can be used as a power of multiplexed metabolic biomarkers was developed by Yu
source. The system could operate using both MFC non-human- and co-workers.[40] This e-skin harvested human sweat energy
inhabiting ammonia-oxidizing bacteria and human-skin-inhab- using lactate biofuel cells and enabled multiplexed monitoring
iting sweat-eating bacteria. Other biodegradable e-skins that of important metabolic biomarkers such as pH, urea, glucose,
operate on a self-power strategy have been described in pre- and NH4+ ion. In this e-skin, the obtained information is trans-
vious sections.[21,273] mitted to the UI via BLE. Byun et al.[294] developed an e-skin
that enabled wirelessly activated soft robots. The described
system was composed of two-part e-skins, which were designed
5.3. Communication and Connectivity to operate by wireless communication of the four-state control
signal “wireless inter-skin communication,” and activated the
Data communication is another challenge in the fabrication of robot when mounted onto each soft body frame (robot and
efficient, biodegradable flexible materials. There are shortcom- human). This e-skin design was thin (<1 mm), soft, and light-
ings regarding the use of wires in biodegradable sensors, such weight (≈0.8 g), reduced the local inherent hardness arising
as potentially causing infections and requiring a secondary from chip-scale components, and could be softly integrated
operation to remove the nonbiodegradable components from into soft body frames. It is worth mentioning that the recent
partially biodegradable sensors and substrates. Thus, wireless high-performance electrodes, circuits, powering, and transmis-
data communication can overcome the limitations of traditional sion units can be integrated into the fully biodegradable e-skin
sensors. However, wireless platforms are generally produced platform using biodegradable conductive, semiconductive, and
from nonbiodegradable or partially biodegradable materials. dielectric components such as PCL, PLLA, PLA, PGS, Mg con-
Therefore, a need exists to develop a fully biodegradable wire- ductors, Si semiconductors, silk or cellulose substrates, and
less platform. In Section 2.2.4, we discussed some biodegrad- SiO2 or MgO dielectric materials.
able e-skins and sensing platforms, which operated based on
wireless sensing mechanisms such as wireless fringe-field
capacitor technology.[30] 5.4. Cytotoxicity
In 2021, Rogers and co-workers[291] introduced long-range
wireless soft electronics for skin hydration monitoring, which Cytotoxicity is the degree to which a chemical substance or com-
provided rapid, efficient, high-sampling-rate, and long-range pound can devastate a cell.[295] The toxicity of a substance to
automated measurements of thermal transport properties. The living cells depends on extrinsic parameters including chemical
reported platform used a miniaturized multisensor module, composition, shape, surface, solubility, size, aggregation, and
which was controlled by a long-range (≈10 m) Bluetooth Low structure.[295] Different types of engineered nanomaterials with
Energy (BLE) on a chip (SoC) for wireless data communication distinctive size, shape, composition, physical, electrical, and mor-
with a user interface (UI) system on a standard smartphone. phological characteristics have been incorporated into the flexible
This device facilitated soft skin contact and quantitative analysis wearable electronics and e-skin based on their unique physico-
of hydration levels of both the epidermis and dermis. The fabri- chemical properties. With such an increase in e-skins containing
cated device was small and designed for noninvasive analysis of nanomaterials, there is a need to understand the cytotoxicity,
the thermal transport properties and temperature of the skin. genotoxicity, and their potential impacts on the environment.
In addition, the application of wireless e-tattoo technology for In general, the cytotoxicity mechanism of nanomaterials
personalized sensing was reported.[292] These e-tattoos were involves three routes including 1) direct association of nano-
composed of a multilayer stack of stretchable layers, in which materials with the surface organism’s cell, 2) Releasing toxic
a near-field communication (NFC) layer facilitated wireless data ions by organism dissolution due to the enzymatic reactions or
transmission and power harvesting. The wireless power and interaction with a cell’s DNA, and 3) the ROS generation and
data transmission via NFC provided an efficient solution that oxidative stress that can damage organism genetic materials.[296]
removed the bulky batteries and electronics, resulting in e-tat- Therefore, to mitigate the cytotoxic impact of nanomaterials
toos with low thickness and high stretchability. In one study, redesigning strategies should be considered. The redesigning
Palmroth et al.[293] investigated the performance and orthopedic strategies for mentioned cytotoxicity pathways include route (1)
applications of wireless inductor–capacitor resonance sensors controlling the shape of nanomaterials, incorporating negatively
prepared using bioresorbable and biodegradable materials, charged ions, and using stealth ligands, route (2) replacing toxic
such as Mg. This Mg-based pressure sensor was wirelessly elements with more benign elements, using shell materials,
readable and pressure-responsive for 10 days under aqueous shape controlling, and chelation, and route (3) tuning of band-
conditions. The sensitivity and resonance frequency drifted gaps, using shell materials, and using antioxidant ligands.[296]
To reduce or eliminate the risk of toxicity for incorporation to decrease the toxicity of MXenes involves the coating with
of nanomaterials in wearable electronics and e-skin various biopolymers that can stabilize the particles and increase the cel-
strategies have been proposed. The MWCNTs and SWCNTs lular uptake. Another strategy includes modification of MXene
have been used widely in the development of e-skins because surface properties by conjugating with biopolymers. Recent
of their unique characteristics such as high electrical conduc- studies suggested coating the biodegradable synthetic and nat-
tivity, exceptional thermal conductivity, and mechanical robust- ural biopolymers such as PLGA, chitosan, poly(l-Lysine), col-
ness.[297] The SWCNT and MWCNT deposition on exposed skin lagen, and SF can decrease the toxicity and enhance the bio-
resulted in active interaction, initiation of oxidative stress in compatibility of MXene.[308–312] In this regard, Wang et al.[312]
the skin, and induction of redox-sensitive transcription factors developed a flexible SF@Ti3C2Tx MXene (SF@MXene) biocom-
thereby affecting/leading to skin inflammation.[298–300] Exposure posite films based on natural SF as a bridging agent between
of mice to SWCNT led to the generation of oxidative stress, glu- (2D) MXene nanosheets. The results confirmed the long-term
tathione depletion, oxidation of protein thiols and carbonyls, biocompatibility of the SF@MXene film in vitro for culturing
myeloperoxidase activity elevation, dermal cell number increase, of SF@MXene on human skin fibroblast–HSAS1 cells. In par-
polymorphonuclear leukocytes accumulation, and skin thick- ticular, the survival rates of human skin fibroblasts-HSAS1
ening.[301] In addition, the application of a low concentration of were 99.5% ± 0.8%, after 6 d (144 h), which showed the SF@
MWCNTs induced the keratinocyte cytotoxicity and exacerba- MXene film was safe for skin contact. In 2022, Liu et al.[313]
tion of allergic skin conditions.[283–285] However, the use of soni- developed an e-skin based on a 2,2,6,6-tetramethylpiperidinyl-
cation and dispersive agents led to the prevention of cytotoxic 1-oxyl (TEMPO)-oxidized cellulose nanofibril (TOCN) disper-
events of MWCNTs exposure in human skin.[299] Approaches sion and highly conductive Ti3C2Tx. To ensure the non-toxicity
to control skin toxicity include encapsulation with benign of developed composite materials, the TOCN/Ti3C2Tx e-skin
materials, using shell components or ligands, and embedding was tested with the L929 cells, which exhibited the existence of
in biocompatible hydrogels. In 2020, Xu et al.[302] developed a a spindle shape in the culture medium and the relative growth
piezoresistive e-skin based on sulfonated multi-walled carbon rate value of TOCN/Ti3C2Tx exceeded 100% after 72 h of cell
nanotubes (SCNT) and 2,2,6,6-tetramethylpiperidinyl-1-oxyl culture. These results confirmed the healthy growth state of
(TEMPO)-oxidized cellulose nanofibrils (TOCNs). The authors cells and biocompatibility of developed e-skin. The biodegrad-
evaluated the biocompatibility of the TOCN/SCNT hydrogel able PLA thin sheets have also been used in combination with
film by performing an in vitro cytotoxicity using L929 cells cul- MXene-impregnated tissue paper to fabricate a biocompatible
tured for 24, 48, and 72 h. The result showed the presence of and biodegradable e-skin.[284] The authors assessed the toxicity
spindle-shaped morphology, indicating that the cells were in a of the sensor using L929 cells cultured for 24, 48, and 72 h.
healthy growth state and no significant toxicity was observed. In Results exhibited the formation of spindle-shaped morphology,
another work, a flexible, biocompatible e-skin based on coating indicating the healthy growth state of the cells, which con-
the CNT with regenerated cellulose (RC)–CNT was reported.[303] firmed the sensor was biocompatible with no observable cyto-
The developed e-skin did not show in vitro cytotoxicity and toxicity. Also, other noteworthy environmentally friendly and
RC-CNT e-skin was non-cytotoxic to mouse fibroblast cell lines biodegradable polymers including poly(N-isopropylacrylamide)
(L929) and exhibited good cell compatibility. In addition, an (pNIPAM), PVA, and PDA were used for coating and function-
e-skin was prepared[158] based on the mesoscopic functionaliza- alizing Ag nanoparticles, AgNWs, and halloysite nanotube with
tion of cocoon silk by incorporating WK and CNTs via an inter- no sign of obvious or severe toxicity in biological cells.[314–316]
molecular templated nucleation strategy. Calcein-stained mouse
preosteoblast-like cells were cultured on both sides (front/back)
of the film. After 2 days, more cells were observed on the front 6. Conclusions and Future Perspectives
than the back (the back-side had more CNTs than the front-side
film) indicating that the front-side of the film with fewer CNTs This review provides an in-depth and comprehensive analysis
was more favorable for the preosteoblasts proliferation. Also, of emerging biodegradable e-skins. This review not only dis-
the authors confirmed both sides’ biocompatibility of developed cussed the recent progress and advances in the field of biode-
e-skin. One biocompatible hybrid hydrogel was developed by gradable skins but also provided readers with a comprehensive
coating SWCNTs using PVA and PDA.[304] The result suggested understanding of biological skin functions and various types
that the hydrogel exhibited no cytotoxicity and could facilitate of transduction mechanisms necessary for the development of
cell attachment and proliferation. The L929 cells cultured in biodegradable e-skins.
extract substrates of the PVA-FSWCNT-PDA hydrogel exhib-
ited the formation of fusiform morphology, which indicated the
healthy growth state of L929 cells. 6.1. Perception, Recognition, and Discrimination
The MXenes have received significant interest because of
graphene-like characteristics, high conductivity, high surface The first part of this review discussed the biological skin sen-
area, hydrophilicity, photothermal conversion, and mechan- sory networks of glabrous and hairy skins, including an activity
ical robustness.[305] Despite the increasing interest in utilizing map of various stimuli and corresponding cells for interpreting
MXene for a wide range of applications, a limited number of in and transmitting signals from human skin to the thalamus
vitro and in vivo investigations on the MXene cytotoxicity were and the cortex, which is a primary step toward designing high-
reported. Previous reports confirmed the role of direct contact performance and ultrasensitive e-skins. The somatosensory
and ROS generation in MXene cytotoxicity.[306,307] One strategy system of biological skin interprets and analyzes various types
of tactile stimuli that provide significant cognitive capabili- 6.2. Biodegradability in Sensors, HMIs, and Robotics
ties for environment recognition. Understanding the physics,
design, and mechanisms and applying the relevant knowledge Human daily life becomes more integrated with the assistance
have improved the fabrication approaches and performance and presence of various electronics, ranging from ubiquitous
efficiencies of next-generation wearable sensors and have pro- personal smartphones to point-of-care (POC) diagnostic smart
vided supplementary and complementary sensing strategies biomedical platforms. In 2019, 53.6 million metric tons (Mt)
for the development of e-skins. The hairy-skin electronics were of e-waste were produced worldwide, a 21% increase in just 5
developed to enable multimodal and airflow detection using an years.[320] A new report predicts that global e-waste production
array of graphene nanoplatelets and artificial microhairs, which will reach 74 Mt by 2030, which is almost double the e-waste
mimicked the functions of biological hairs.[317] The reported production just 16 years earlier. In 2019, only 17.4% of e-waste
platform with percolated networks of graphene nanoplatelet was collected and recycled, which led to the dumping and
sheets could detect the spatial distribution of applied pressures burning of valuable Au, Ag, Cu, Pt, and other rare-earth metals,
with localized temperature differences, similar to biological valued at US $57 billion.[320] In this regard, “green electronics”
skin. Another example of this category includes the bendable and the development of biodegradable components for elec-
biomimetic whisker mechanoreceptor as a TENG-based, self- tronics are essential steps toward the efficient management of
powered, low-cost, and sensitive hair-based sensor for robotic e-waste. Natural biopolymers such as cellulose, chitosan, starch,
tactile sensing applications.[318] Because of the leverage effect of fibroin, and collagen have provided attractive building blocks for
the whisker, the platform could distinguish between weak envi- the fabrication of next-generation flexible, biocompatible, and
ronmental disturbances (1.129 µN), which provided tactile sen- biodegradable e-skins, which will endow e-skins with high effi-
sitivity to robotic systems for environmental detection. ciency, low cost, low density, high abundance, high availability,
In the second part of this review, we discussed the main and environmental benignity. The stability, exceptional tensile
transduction mechanisms developed in e-skins, focusing on strength,[321] unique optical characteristics, biocompatibility,
biodegradable e-skins. Most importantly, this section surveyed and biodegradability of cellulose have inspired the development
other recent transduction mechanisms, including TENG and of various integrated biodegradable and biocompatible e-skins.
combined TENG/PENG approaches, chemomechanical trans- However, the limitations of cellulose, which include low con-
duction, mechanotransduction, and multimodal approaches ductivity, low stretchability, and structural complexity, are major
based on various electrical characteristics of piezoelectricity, pie- drawbacks to the widespread application of cellulose in e-skins.
zoresistivity, and triboelectricity. Comparing conventional trans- SF exhibits the advantages of high mechanical robustness,
duction mechanisms with other hybrid or novel mechanisms solution-processability, easy deformability, easy modification,
is extremely important in understanding the physical and and programmable degradation, and these advantages make SF
chemical characteristics of e-skins and providing readers with a desirable material for use in analytical sciences, electronics,
basic knowledge to develop and fabricate high-performance and biomedical engineering.[322–324] Despite the advantages of
future-generation e-skins. For example, the potentiometric SF, its poor extensibility and tendency to thermally degrade
mechanotransduction mechanism[319] was developed based on a limit its applications at high operating temperatures. In 2020,
measured mechanically regulated potential difference between an e-skin based on a heat-resistant and mechanically robust
two electrodes that encoded the mechanical stimuli as potential SF composite membrane was developed.[325] The reported
difference variations. The reported device based on this mecha- e-skin exhibited excellent extensibility (>200%), high transmit-
nism does not rely on external power sources and exhibits an tance (>90%), air permeability (21.2 mm s−1), and enhanced
ultralow power consumption of less than 1 nW, which is sev- heat resistance (to 160 °C). Inkjet printing was used to con-
eral orders of magnitude lower than the power consumption of struct Ag and Pt nanofiber networks on both sides of the SF
other conventional platforms. In addition, the potentiometric composite membranes to function as heaters and temperature
mechanotransducer detected both static and low-frequency sensors, respectively. The Ag nanofiber network exhibited high
dynamic mechanical stimuli, mitigating the limitations of self- thermal resistance, high tensile stability, and heating cyclicity,
powered triboelectric and piezoelectric platforms for recording whereas the Pt nanofiber network exhibited a short response
static mechanical stimuli. Because of these advantages, mecha- time (<2 s) and high temperature sensitivity (0.205% °C−1). The
notransduction could be a cornerstone to understanding the promising characteristics of biodegradable biopolymers could
nature and performance of stretchable, soft, and multifunc- reshape and redefine the design of next-generation e-skins
tional e-skins. Recently, a stretchable multimodal e-skin that toward environmental sustainability and benignity, spurring
operated on various mechanisms including triboelectricity, pie- the development of highly sensitive, programmable, and biode-
zoelectricity, and piezoresistivity was introduced.[5] This device gradable e-skins, which could have a revolutionary impact on
exceeds the tactile perception capabilities of biological skins and society and the scientific community. Other than the natural
can identify and distinguish mechanical stresses from a combi- biopolymers, there are noteworthy biocompatible and biode-
nation of multiple stimuli. The use of AgNWs and ZnO NWs gradable synthetic polymers, such as PHB, PCL, PLA, poly(3-
not only imparts hybrid piezoresistive, triboelectric, and piezo- hydroxyoctanoate), poly(glycolide-co-caprolactone), poly(glycolic
electric characteristics but also achieves stimulus discrimina- acid), PLLA, poly(1,8-octanediol-cocitrate), poly(l-lactide-co-
bility by fitting specific signals to specific stimuli. The reported ε-caprolactone), poly(l-lactide), POMaC and PGS, which have
device can perceive material substances, surface energy, surface been discussed and explored in similar applications. The bio-
charge density, and roughness, providing a unique platform for degradable characteristics of e-skins can be improved by fabri-
applications in HMIs, prosthetics, sensors, and robotics. cation of electrodes using environmentally friendly non-noble
metals such as Mg and Fe that can be degraded in water or Keywords

mild acid/base solutions. In addition, modification of the mate-
biodegradability, electronic skins, health monitoring, human–machine
rial’s chemical structure by the introduction of polar function-
interfaces, sensing, wearable electronics
alities can enhance the biodegradability and solubility of e-skin
in non-toxic and biorenewable green solvents. Received: April 8, 2022
Development of biodegradable wireless powering and com- Revised: June 13, 2022
munication units is essential to fabricate reliable biodegradable Published online: November 30, 2022
and biocompatible e-skins. In this regard, various biodegradable
supercapacitors, energy harvesters, batteries, and photovoltaic cells
have been introduced. However, the incorporation of these units
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Mohammad Zarei received his Ph.D. degree in physical chemistry from Ferdowsi University of
Mashhad in 2016. He is currently a postdoctoral fellow at University of Ulsan, Department of
Chemistry. His current research focuses on the biomedical applications of polymer nanocompos-
ites, electronic skins, point-of-care diagnostics, and high-performance portable sensing platforms
for resource-limited settings. Recently, he is expanding his research on developing biodegradable
electronic skins for the potential application in sensing, robotics, and human–machine interfaces.
Seung Goo Lee is an Assistant Professor in the Department of Chemistry at University of Ulsan,
Korea. He received his B.S. degree (2006) in chemical engineering from Hanyang University and
his Ph.D. degree (2012) in chemical engineering from POSTECH. After that, he was a postdoc-
toral researcher at POSTECH (2012–2014) and MIT (2014–2016). Before joining University of
Ulsan, he worked as a senior engineer at Samsung Electronics (2016–2018). His research inter-
ests include bioinspired polymer materials and surface/interface engineering for soft electronics.
Kilwon Cho is a University Professor in the Department of Chemical Engineering and director of
the Polymer Research Institute at POSTECH, Korea. He received his B.S. and M.S. degrees from
Seoul National University in applied chemistry and his Ph.D. degree (1986) from the University of
Akron in polymer science. After working as a researcher at the IBM Research Center, he joined the
faculty at POSTECH (1988). His research interests include polymer surfaces, interfaces and thin
films, organic semiconductor materials and optoelectronic properties, and surface and interface
engineering of 2D materials and soft electronics.

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Advances in Biodegradable Electronic Skin: Material

strain. The signals generated by these

The conventional transduction mechanisms offered advantages

Materials Mechanism Sensitivity & Performance Degradation Ref Application

metals such as Mg and Fe that can be degraded in water or Keywords

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