Wearable,Healable, and Adhesive Epidermal Sensors Assembled from Mussel‐Inspired Conductive Hybrid Hydrogel Framework

Healable, adhesive, wearable, and soft human‐motion sensors for ultrasensitive human–machine interaction and healthcare monitoring are successfully assembled from conductive and human‐friendly hybrid hydrogels with reliable self‐healing capability and robust self‐adhesiveness. The conductive, healable, and self‐adhesive hybrid network hydrogels are prepared from the delicate conformal coating of conductive functionalized single‐wall carbon nanotube (FSWCNT) networks by dynamic supramolecular cross‐linking among FSWCNT, biocompatible polyvinyl alcohol, and polydopamine. They exhibit fast self‐healing ability (within 2 s), high self‐healing efficiency (99%), and robust adhesiveness, and can be assembled as healable, adhesive, and soft human‐motion sensors with tunable conducting channels of pores for ions and framework for electrons for real time and accurate detection of both large‐scale and tiny human activities (including bending and relaxing of fingers, walking, chewing, and pulse). Furthermore, the soft human‐motion sensors can be enabled to wirelessly monitor the human activities by coupling to a wireless transmitter. Additionally, the in vitro cytotoxicity results suggest that the hydrogels show no cytotoxicity and can facilitate cell attachment and proliferation. Thus, the healable, adhesive, wearable, and soft human‐motion sensors have promising potential in various wearable, wireless, and soft electronics for human–machine interfaces, human activity monitoring, personal healthcare diagnosis, and therapy.     

Highly Elastic Graphene‐Based Electronics Toward Electronic Skin

Epidermal electronics are extensively explored as an important platform for future biomedical engineering. Epidermal devices are typically fabricated using high‐cost methods employing complex vacuum microfabrication processes, limiting their widespread potential in wearable electronics. Here, a low‐cost, solution‐based approach using electroconductive reduced graphene oxide (RGO) sheets on elastic and porous poly(dimethylsiloxane) (PDMS) thin films for multifunctional, high‐performance, graphene‐based epidermal bioelectrodes and strain sensors is presented. These devices are fabricated employing simple coatings and direct patterning without using any complicated microfabrication processes. The graphene bioelectrodes show a superior stretchability (up to 150% strain), with mechanical durability up to 5000 cycles of stretching and releasing, and low sheet resistance (1.5 kΩ per square), and the graphene strain sensors exhibit a high sensitivity (a gauge factor of 7 to 173) with a wide sensing range (up to 40% strain). Fully functional applications of dry bioelectrodes in monitoring human electrophysiological signals (i.e., electrocardiogram, electroencephalography, and electromyogram) and highly sensitive strain sensors for precise detection of large‐scale human motions are demonstrated. It is believed that our unique processing capability and multifunctional device platform based on RGO/porous PDMS will pave the way for low‐cost processing and integration of 2D materials for future wearable electronic skin.     

Large‐Area Ultrathin Graphene Films by Single‐Step Marangoni Self‐Assembly for Highly Sensitive Strain Sensing Application

Promoted by the demand for wearable devices, graphene has been proved to be a promising material for potential applications in flexible and highly sensitive strain sensors. However, low sensitivity and complex processing of graphene retard the development toward the practical applications. Here, an environment‐friendly and cost‐effective method to fabricate large‐area ultrathin graphene films is proposed for highly sensitive flexible strain sensor. The assembled graphene films are derived rapidly at the liquid/air interface by Marangoni effect and the area can be scaled up. These graphene‐based strain sensors exhibit extremely high sensitivity with gauge factor of 1037 at 2% strain, which represents the highest value for graphene platelets at this small deformation so far. This simple fabrication for strain sensors with highly sensitive performance of strain sensor makes it a novel approach to applications in electronic skin, wearable sensors, and health monitoring platforms.     

Polyelectrolyte Dielectrics for Flexible Low‐Voltage Organic Thin‐Film Transistors in Highly Sensitive Pressure Sensing

Organic thin‐film transistors (OTFTs) can provide an effective platform to develop flexible pressure sensors in wearable electronics due to their good signal amplification function. However, it is particularly difficult to realize OTFT‐based pressure sensors with both low‐voltage operation and high sensitivity. Here, controllable polyelectrolyte composites based on poly(ethylene glycol) (PEG) and polyacrylic acid (PAA) are developed as a type of high‐capacitance dielectrics for flexible OTFTs and ultrasensitive pressure sensors with sub‐1 V operation. Flexible OTFTs using the PAA:PEG dielectrics show good universality and greatly enhanced electrical performance under a much smaller operating voltage of ?0.7 V than those with a pristine PAA dielectric. The low‐voltage OTFTs also exhibit excellent flexibility and bending stability under various bending radii and long cycles. Flexible OTFT‐based pressure sensors with low‐voltage operation and superhigh sensitivity are demonstrated by using a suspended semiconductor/dielectric/gate structure in combination with the PAA:PEG dielectric. The sensors deliver a record high sensitivity of 452.7 kPa^?1 under a low‐voltage of ?0.7 V, and excellent operating stability over 5000 cycles. The OTFT sensors can be built into a wearable sensor array for spatial pressure mapping, which shows a bright potential in flexible electronics such as wearable devices and smart skins.     

Wearable and Implantable Triboelectric Nanogenerators

Triboelectric nanogenerators (TENGs) are a promising technology to convert mechanical energy to electrical energy based on coupled triboelectrification and electrostatic induction. With the rapid development of functional materials and manufacturing techniques, wearable and implantable TENGs have evolved into playing important roles in clinic and daily life from in vitro to in vivo. These flexible and light membrane‐like devices have the potential to be a new power supply or sensor element, to meet the special requirements for portable electronics, promoting innovation in electronic devices. In this review, the recent advances in wearable and implantable TENGs as sustainable power sources or self‐powered sensors are reviewed. In addition, the remaining challenges and future possible improvements of wearable and implantable TENG‐based self‐powered systems are discussed.     

A Dual‐Functional Graphene‐Based Self‐Alarm Health‐Monitoring E‐Skin

Diseases such as cardiovascular problems and sleep apnea cause mass deaths annually due to a lack of timely and portable monitoring and alarm measures. Various wearable devices for health monitoring have been intensely researched to reduce mortality. However, these devices themselves can only detect physiological signals; they cannot sound an alarm. Therefore, they must rely on mobile phones or other peripheral devices such as speakers or vibration motors to sound an alarm, which may result in a patient missing the optimal treatment. It is valuable to develop a self‐alarm health monitoring device with the dual functions of physiological signal detection and sound alarm simultaneously. A one‐step laser‐induced graphene (LIG)‐based electronic skin (E‐skin) is fabricated to perform health monitoring and alarm at the same time, which benefit from its both excellent mechanical and acoustical performance. These customized shutter‐patterned E‐skins have an ultrahigh sensitivity of 316.3 and can detect various biosignals such as wrist pulse, respiratory, etc. They also have a self‐alarm function and can sound an alarm when detecting abnormal situations. This study addresses the multifunctional integration required for multisensors, which will open further applications in wearable sensors and health‐care devices.     

Emerging Wearable Sensors for Plant Health Monitoring

Emerging plant diseases, caused by pathogens, pests, and climate change, are critical threats to not only the natural ecosystem but also human life. To mitigate crop loss due to various biotic and abiotic stresses, new sensor technologies to monitor plant health, predict, and track plant diseases in real time are desired. Wearable electronics have recently been developed for human health monitoring. However, the application of wearable electronics to agriculture and plant science is in its infancy. Wearable technologies mean that the sensors will be directly placed on the surfaces of plant organs such as leaves and stems. The sensors are designed to detect the status of plant health by profiling various trait biomarkers and microenvironmental parameters, transducing bio-signals to electric readout for data analytics. In this perspective, the recent progress in wearable plant sensors is summarized and they are categorized by the functionality, namely plant growth sensors, physiology, and microclimate sensors, chemical sensors, and multifunctional sensors. The design and mechanism of each type of wearable sensors are discussed and their applications to address the current challenges of precision agriculture are highlighted. Finally, challenges and perspectives for the future development of wearable plant sensors are presented.     

Materials for Printable,Transparent, and Low‐Voltage Transistors

Since the 1990s, printable, transparent, and low‐voltage transistors have attracted great attention from academia and industry due to the demand for specialized circuitry such as in radio‐frequency identification (RFID) tags, medical sensors, and electronically active textiles. Some flexible and portable devices have been available commercially; however, the challenge to convert more conceptual devices into real‐life applications is still the materials. This article starts with a brief summary of some examples from silicon electronics, to place the other materials in context, followed by the topics including high‐capacitance dielectrics, transparent conductors and semiconductors, and printability of recently developed electronic materials. The recent progress about these topics is reviewed, and discussions of each topic suggest future science and engineering research opportunities.     

Stretchable,Skin‐Mountable,and Wearable Strain Sensors and Their Potential Applications: A Review

There is a growing demand for flexible and soft electronic devices. In particular, stretchable, skin‐mountable, and wearable strain sensors are needed for several potential applications including personalized health‐monitoring, human motion detection, human‐machine interfaces, soft robotics, and so forth. This Feature Article presents recent advancements in the development of flexible and stretchable strain sensors. The article shows that highly stretchable strain sensors are successfully being developed by new mechanisms such as disconnection between overlapped nanomaterials, crack propagation in thin films, and tunneling effect, different from traditional strain sensing mechanisms. Strain sensing performances of recently reported strain sensors are comprehensively studied and discussed, showing that appropriate choice of composite structures as well as suitable interaction between functional nanomaterials and polymers are essential for the high performance strain sensing. Next, simulation results of piezoresistivity of stretchable strain sensors by computational models are reported. Finally, potential applications of flexible strain sensors are described. This survey reveals that flexible, skin‐mountable, and wearable strain sensors have potential in diverse applications while several grand challenges have to be still overcome.     

Flexible MXene-Based Composites for Wearable Devices

In recent decades, flexible and wearable devices have been extensively investigated due to their promising applications in portable mobile electronics and human motion monitoring. MXene, a novel growing family of 2D nanomaterials, demonstrates superiorities such as outstanding electrical conductivity, abundant terminal groups, unique layered-structure, large surface area, and hydrophilicity, making it to be a potential candidate material for flexible and wearable devices. Numerous pioneering works are devoted to develop flexible MXene-based composites with various functions and designed structures. Therefore, the latest progress of the flexible MXene-based composites for wearable devices is summarized in this review, focusing on the preparation strategies, working mechanisms, performances, and applications in sensors, supercapacitors, and electromagnetic interference shielding materials. Moreover, the current challenges and future outlooks are also discussed.     

Porous Fibers Composed of Polymer Nanoball Decorated Graphene for Wearable and Highly Sensitive Strain Sensors

Wearable textile strain sensors that can perceive and respond to human stimuli are an essential part of wearable electronics. Yet, the detection of subtle strains on the human body suffers from the low sensitivity of many existing sensors. Generally, the inadequate sensitivity originates from the strong structural integrity of the sensors because tiny external strains cannot trigger enough variation in the conducting network. Inspired by the rolling friction where the interaction is weakened by decreasing interface area, porous fibers made of graphene decorated with nanoballs are prepared via a prolonged phase‐separation process. This novel structure confers the graphene fibers with high gauge factors (51 in 0–5% and 87 in 5–8%), which is almost 10 times larger than the same structures without nanoballs. A low detection limit (0.01% strain) and good durability (over 6000 circles) are obtained. By the virtue of these qualities, these fiber‐based textile sensors can recognize a pulse wave and eyeball movement in real‐time while keeping comfortable wearing sense. Moreover, by weaving such fibers, the electronic fabrics with a specially designed structure can distinguish the multilocation in real time, which shows great potential as wearable electronics.     

Flexible and Highly Sensitive Strain Sensors Fabricated by Pencil Drawn for Wearable Monitor

Functional electrical devices have promising potentials in structural health monitoring system, human‐friendly wearable interactive system, smart robotics, and even future multifunctional intelligent room. Here, a low‐cost fabrication strategy to efficiently construct highly sensitive graphite‐based strain sensors by pencil‐trace drawn on flexible printing papers is reported. The strain sensors can be operated at only two batteries voltage of 3 V, and can be applied to variously monitoring microstructural changes and human motions with fast response/relaxation times of 110 ms, a high gauge factor (GF) of 536.6, and high stability >10 000 bending–unbending cycles. Through investigation of service behaviors of the sensors, it is found that the microcracks occur on the surface of the pencil‐trace and have a major influence on the functions of the strain sensors. These performances of the strain sensor attain and even surpass the properties of recent strain sensing devices with subtle design of materials and device architectures. The pen‐on‐paper (PoP) approach may further develop portable, environmentally friendly, and economical lab‐on‐paper applications and offer a valuable method to fabricate other multifunctional devices.     

Ionic Tactile Sensors for Emerging Human‐Interactive Technologies: A Review of Recent Progress

Ionic tactile sensors (ITS) represent a new class of deformable sensory platforms that mimic not only the tactile functions and topological structures but also the mechanotransduction mechanism across the biological ion channels in human skin, which can demonstrate a more advanced biological interface for targeting emerging human‐interactive technologies compared to conventional e‐skin devices. Recently, flexible and even stretchable ITS have been developed using novel structural designs and strategies in materials and devices. These skin‐like tactile sensors can effectively sense pressure, strain, shear, torsion, and other external stimuli with high sensitivity, high reliability, and rapid response beyond those of human perception. In this review, the recent developments of the ITS based on the novel concepts, structural designs, and strategies in materials innovation are entirely highlighted. In particular, biomimetic approaches have led to the development of the ITS that extend beyond the tactile sensory capabilities of human skin such as sensitivity, pressure detection range, and multimodality. Furthermore, the recent progress in self‐powered and self‐healable ITS, which should be strongly required to allow human‐interactive artificial sensory platforms is reviewed. The applications of ITS in human‐interactive technologies including artificial skin, wearable medical devices, and user‐interactive interfaces are highlighted. Last, perspectives on the current challenges and the future directions of this field are presented.     

Hybrid Smart Fiber with Spontaneous Self‐Charging Mechanism for Sustainable Wearable Electronics

Smart wearable electronics that are fabricated on light‐weight fabrics or flexible substrates are considered to be of next‐generation and portable electronic device systems. Ideal wearable and portable applications not only require the device to be integrated into various fiber form factors, but also desire self‐powered system in such a way that the devices can be continuously supplied with power as well as simultaneously save the acquired energy for their portability and sustainability. Nevertheless, most of all self‐powered wearable electronics requiring both the generation of the electricity and storing of the harvested energy, which have been developed so far, have employed externally connected individual energy generation and storage fiber devices using external circuits. In this work, for the first time, a hybrid smart fiber that exhibits a spontaneous energy generation and storage process within a single fiber device that does not need any external electric circuit/connection is introduced. This is achieved through the employment of asymmetry coaxial structure in an electrolyte system of the supercapacitor that creates potential difference upon the creation of the triboelectric charges. This development in the self‐charging technology provides great opportunities to establish a new device platform in fiber/textile‐based electronics.     

Wearable Force Touch Sensor Array Using a Flexible and Transparent Electrode

Transparent electrodes have been widely used for various electronics and optoelectronics, including flexible ones. Many nanomaterial‐based electrodes, in particular 1D and 2D nanomaterials, have been proposed as next‐generation transparent and flexible electrodes. However, their transparency, conductivity, large‐area uniformity, and sometimes cost are not yet sufficient to replace indium tin oxide (ITO). Furthermore, the conventional ITO is quite rigid and susceptible to mechanical fractures under deformations (e.g., bending, folding). In this study, the authors report new advances in the design, fabrication, and integration of wearable and transparent force touch (touch and pressure) sensors by exploiting the previous efforts in stretchable electronics as well as novel ideas in the transparent and flexible electrode. The optical and mechanical experiment, along with simulation results, exhibit the excellent transparency, conductivity, uniformity, and flexibility of the proposed epoxy‐copper‐ITO (ECI) multilayer electrode. By using this multi‐layered ECI electrode, the authors present a wearable and transparent force touch sensor array, which is multiplexed by Si nanomembrane p‐i‐n junction‐type (PIN) diodes and integrated on the skin‐mounted quantum dot light‐emitting diodes. This novel integrated system is successfully applied as a wearable human–machine interface (HMI) to control a drone wirelessly. These advances in novel material structures and system‐level integration strategies create new opportunities in wearable smart displays.     

On‐Body Bioelectronics: Wearable Biofuel Cells for Bioenergy Harvesting and Self‐Powered Biosensing

The growing power demands of wearable electronic devices have stimulated the development of on‐body energy‐harvesting strategies. This article reviews the recent progress on rapidly emerging wearable biofuel cells (BFCs), along with related challenges and prospects. Advanced on‐body BFCs in various wearable platforms, e.g., textiles, patches, temporary tattoo, or contact lenses, enable attractive advantages for bioenergy harnessing and self‐powered biosensing. These noninvasive BFCs open up unique opportunities for utilizing bioenergy or monitoring biomarkers present in biofluids, e.g., sweat, saliva, interstitial fluid, and tears, toward new biomedical, fitness, or defense applications. However, the realization of effective wearable BFC requires high‐quality enzyme‐electronic interface with efficient enzymatic and electrochemical processes and mechanical flexibility. Understanding the kinetics and mechanisms involved in the electron transfer process, as well as enzyme immobilization techniques, is essential for efficient and stable bioenergy harvesting under diverse mechanical strains and changing operational conditions expected in different biofluids and in a variety of outdoor activities. These key challenges of wearable BFCs are discussed along with potential solutions and future prospects. Understanding these obstacles and opportunities is crucial for transforming traditional bench‐top BFCs to effective and successful wearable BFCs.     

Flexible Piezoresistive Sensor Patch Enabling Ultralow Power Cuffless Blood Pressure Measurement

Noninvasive and real‐time cuffless blood pressure (BP) measurement realizes the idea of unobtrusive and continuous BP monitoring which is essential for diagnosis and prevention of cardiovascular diseases associated with hypertension. In this paper, a wearable sensor patch system that integrates flexible piezoresistive sensor (FPS) and epidermal electrocardiogram (ECG) sensors for cuffless BP measurement is presented. By developing parametric models on the FPS sensing mechanism and optimizing operational conditions, a highly stable epidermal pulse monitoring method is established and beat‐to‐beat BP measurement from the ECG and epidermal pulse signals is demonstrated. In particular, this study highlights the compromise between sensor sensitivity and signal stability. As compared with the current optical‐based cuffless BP measurement devices, the sensing patch requires much lower power consumption (3 nW) and is capable of detecting subtle physiological signal variations, e.g., pre and postexercises, thus providing a promising solution for low‐power, real‐time, and home‐based BP monitoring.     

Self‐Healing,Flexible, and Tailorable Triboelectric Nanogenerators for Self‐Powered Sensors based on Thermal Effect of Infrared Radiation

Self‐healing triboelectric nanogenerators (TENGs) with flexibility, robustness, and conformability are highly desirable for promising flexible and wearable devices, which can serve as a durable, stable, and renewable power supply, as well as a self‐powered sensor. Herein, an entirely self‐healing, flexible, and tailorable TENG is designed as a wearable sensor to monitor human motion, with infrared radiation from skin to promote self‐healing after being broken based on thermal effect of infrared radiation. Human skin is a natural infrared radiation emitter, providing favorable conditions for the device to function efficiently. The reversible imine bonds and quadruple hydrogen bonding (UPy) moieties are introduced into polymer networks to construct self‐healable electrification layer. UPy‐functionalized multiwalled carbon nanotubes are further incorporated into healable polymer to obtain conductive nanocomposite. Driven by the dynamic bonds, the designed and synthesized materials show excellent intrinsic self‐healing and shape‐tailorable features. Moreover, there is a robust interface bonding in the TENG devices due to the similar healable networks between electrification layer and electrode. The output electric performances of the self‐healable TENG devices can almost restore their original state when the damage of the devices occurs. This work presents a novel strategy for flexible devices, contributing to future sustainable energy and wearable electronics.     

Multiaxial and Transparent Strain Sensors Based on Synergetically Reinforced and Orthogonally Cracked Hetero‐Nanocrystal Solids

Wearable strain sensors are widely researched as core components in electronic skin. However, their limited capability of detecting only a single axial strain, and their low sensitivity, stability, opacity, and high production costs hinder their use in advanced applications. Herein, multiaxially highly sensitive, optically transparent, chemically stable, and solution‐processed strain sensors are demonstrated. Transparent indium tin oxide and zinc oxide nanocrystals serve as metallic and insulating components in a metal–insulator matrix and as active materials for strain gauges. Synergetic sensitivity‐ and stability‐reinforcing agents are developed using a transparent SU‐8 polymer to enhance the sensitivity and encapsulate the devices, elevating the gauge factor up to over 3000 by blocking the reconnection of cracks caused by the Poisson effect. Cross‐shaped patterns with an orthogonal crack strategy are developed to detect a complex multiaxial strain, efficiently distinguishing strains applied in various directions with high sensitivity and selectivity. Finally, all‐transparent wearable strain sensors with Ag nanowire electrodes are fabricated using an all‐solution process, which effectively measure not only the human motion or emotion, but also the multiaxial strains occurring during human motion in real time. The strategies can provide a pathway to realize cost‐effective and high‐performance wearable sensors for advanced applications such as bio‐integrated devices.     

Ultrasensitive and Highly Stretchable Multifunctional Strain Sensors with Timbre‐Recognition Ability Based on Vertical Graphene

Stretchable/wearable strain sensors are attracting growing interest due to their broad applications in physical and physiological measurements. However, the development of a multifunctional highly stretchable sensor satisfying the requirements of ultrahigh sensitivity (able to distinguish sound frequency) remains a challenge. An ultrasensitive and highly stretchable multifunctional strain sensor with timbre‐recognition ability based on high‐crack‐density vertical graphene (VGr) is fabricated using an ultrasonic peeling (UP) method. It can distinguish frequencies of sounds higher than 2500 Hz. Detailed microscopic examinations reveal that their ultrahigh sensitivity stems from the formation of high‐density nanocracks in the graphitic base layer, which is bridged by the top branched VGr nanowalls. These nanocracks cut the VGr film into a large number of nanopieces, which increase the natural frequency of the sensors, enabling the sensors to distinguish the sound frequency. Demonstrations are presented to highlight the sensors' potential as wearable devices for human physiological signal and timbre detections. This is the first multifunctional highly stretchable strain sensor with timbre‐recognition ability.