Free‐Standing and Eco‐Friendly Polyaniline Thin Films for Multifunctional Sensing of Physical and Chemical Stimuli

Multifunctional flexible sensors that are sensitive to different physical and chemical stimuli but remain unaffected by any mechanical deformation and/or changes still present a challenge in the implementation of flexible devices in real‐world conditions. This challenge is greatly intensified by the need for an eco‐friendly fabrication technique suitable for mass production. A new eco‐friendly and scalable fabrication approach is reported for obtaining thin and transparent multifunctional sensors with regulated electrical conductivity and tunable band‐gap. A thin (≈190 nm thickness) freestanding sensing film with up to 4 inch diameter is demonstrated. Integration of the freestanding films with different substrates, such as polyethylene terephthalate substrates, silk textile, commercial polyethylene thin film, and human skin, is also described. These multifunctional sensors can detect and distinguish between different stimuli, including pressure, temperature, and volatile organic compounds. All the sensing properties explored are stable under different bending/strain states.     

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.     

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.     

Biocompatible Soft Fluidic Strain and Force Sensors for Wearable Devices

Fluidic soft sensors have been widely used in wearable devices for human motion capturing. However, thus far, the biocompatibility of the conductive liquid, the linearity of the sensing signal, and the hysteresis between the loading and release processes have limited the sensing quality as well as the applications of these sensors. In this paper, silicone based strain and force sensors composed of a novel biocompatible conductive liquid (potassium iodide and glycerol solution) are introduced. The strain sensors exhibit negligible hysteresis up to 5 Hz, with a gauge factor of 2.2 at 1 Hz. The force sensors feature a novel multifunctional layered structure, with microcylinder‐filled channels to achieve high linearity, low hysteresis (5.3% hysteresis at 1 Hz), and good sensitivity (100% resistance increase at a 5 N load). The sensors' gauge factors are stable at various temperatures and humidity levels. These biocompatible, low hysteresis, and high linearity sensors are promising for safe and reliable diagnostic devices, wearable motion capture, and compliant human–computer interfaces.     

Microporous Polypyrrole‐Coated Graphene Foam for High‐Performance Multifunctional Sensors and Flexible Supercapacitors

This study reports on the fabrication of pressure/temperature/strain sensors and all‐solid‐state flexible supercapacitors using only polydimethylsiloxane coated microporous polypyrrole/graphene foam composite (PDMS/PPy/GF) as a common material. A dual‐mode sensor is designed with PDMS/PPy/GF, which measures pressure and temperature with the changes of current and voltage, respectively, without interference to each other. The fabricated dual‐mode sensor shows high sensitivity, fast response/recovery, and high durability during 10 000 cycles of pressure loading. The pressure is estimated using the thermoelectric voltage induced by simultaneous increase in temperature caused by a finger touch on the sensor. Additionally, a resistor‐type strain sensor fabricated using the same PDMS/PPy/GF could detect the strain up to 50%. Flexible, high performance supercapacitor used as a power supply is fabricated with electrodes of PPy/GF for its high surface area and pseudocapacitance. Furthermore, an integrated system of such fabricated multifunctional sensors and a supercapacitor on a skin‐attachable flexible substrate using liquid–metal interconnections operates well, whereas sensors are driven by the power of the supercapacitor. This study clearly demonstrates that the appropriate choice of a single functional material enables fabrication of active multifunctional sensors for pressure, temperature, and strain, as well as the supercapacitor, that could be used in wirelessly powered wearable devices.     

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.     

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.     

A Highly Stretchable ZnO@Fiber‐Based Multifunctional Nanosensor for Strain/Temperature/UV Detection

Stretchable and multifunctional sensors can be applied in multifunctional sensing devices, safety forewarning equipment, and multiparametric sensing platforms. However, a stretchable and multifunctional sensor was hard to fabricate until now. Herein, a scalable and efficient fabrication strategy is adopted to yield a sensor consisting of ZnO nanowires and polyurethane fibers. The device integrates high stretchability (tolerable strain up to 150%) with three different sensing capabilities, i.e., strain, temperature, and UV. Typically achieved specifications for strain detection are a fast response time of 38 ms, a gauge factor of 15.2, and a high stability of >10 000 cyclic loading tests. Temperature is detected with a high temperature sensitivity of 39.3% °C^?1, while UV monitoring features a large ON/OFF ratio of 158.2. With its fiber geometry, mechanical flexibility, and high stretchability, the sensor holds tremendous prospect for multiparametric sensing platforms, including wearable devices.     

Stretchable and Temperature‐Sensitive Polymer Optical Fibers for Wearable Health Monitoring

Stretchable physical sensors that can detect and quantify human physiological signals such as temperature, are essential to the realization of healthcare devices for biomedical monitoring and human–machine interfaces. Despite recent achievements in stretchable electronic sensors using various conductive materials and structures, the design of stretchable sensors in optics remains a considerable challenge. Here, an optical strategy for the design of stretchable temperature sensors, which can maintain stable performance even under a strain deformation up to 80%, is reported. The optical temperature sensor is fabricated by the incorporation of thermal‐sensitive upconversion nanoparticles (UCNPs) in stretchable polymer‐based optical fibers (SPOFs). The SPOFs are made from stretchable elastomers and constructed in a step‐index core/cladding structure for effective light confinements. The UCNPs, incorporated in the SPOFs, provide thermal‐sensitive upconversion emissions at dual wavelengths for ratiometric temperature sensing by near‐infrared excitation, while the SPOFs endow the sensor with skin‐like mechanical compliance and excellent light‐guiding characteristics for laser delivery and emission collection. The broad applications of the proposed sensor in real‐time monitoring of the temperature and thermal activities of the human body, providing optical alternatives for wearable health monitoring, are demonstrated.     

Flexible and Stretchable Fiber-Shaped Triboelectric Nanogenerators for Biomechanical Monitoring and Human-Interactive Sensing

Wearable, flexible, and even stretchable tactile sensors, such as various types of electronic skin, have attracted extensive attention, which can adapt to complex and irregular surfaces, maximize the matching of wearable devices, and conformally apply onto human organs. However, it is a great challenge to simultaneously achieve breathability, permeability, and comfortability for their development. Herein, mitigating the problem by miniaturizing and integrating the sensors is tried. Highly flexible and stretchable coaxial structure fiber-shaped triboelectric nanogenerators (F-TENGs) with a diameter of 0.63 mm are created by orderly depositing conductive material of silver nanowires/carbon nanotubes and encapsulated polydimethylsiloxane onto the stretchable spandex fiber. As a self-powered multifunctional sensor, the resulting composite fiber can convert mechanical stimuli into electrical signals without affecting the normal human body. Moreover, the F-TENGs can be easily integrated into traditional textiles to form tactile sensor arrays. Through the tactile sensor arrays, the real-time tactile trajectory and pressure distribution can be precisely mapped. This work may provide a new method to fabricate fiber-based pressure sensors with high sensitivity and stretchability, which have great application prospects in personal healthcare monitoring and human–machine interactions.     

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.     

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.     

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.     

Superelastic and Arbitrary‐Shaped Graphene Aerogels with Sacrificial Skeleton of Melamine Foam for Varied Applications

Elastic graphene aerogels are lightweight and offer excellent and electrical performance, expanding their significance in many applications. Recently, elastic graphene aerogels have been fabricated via various methods. However, for most reported elastic graphene aerogels, the fabrication processes are complicated and the applications are usually limited by the brittle mechanical properties. Thus, it still remains a challenge to explore facile processes for the fabrication of graphene aerogels with low density and high compressibility. Herein, arbitrary‐shaped, superelastic, and durable graphene aerogels are fabricated using melamine foam as sacrificial skeleton. The resulting graphene aerogels possess high elasticity under compressive stress of 0.556 MPa and compressive strain of 95%. Thanks to the superelasticity, high strength, excellent flexibility, outstanding thermal stability, and good electrical conductivity of graphene aerogels, they can be applied in sorbents and pressure/strain sensors. The as‐assembled graphene aerogels can adsorb various organic solvents at 176–513 g g^?1 depending on the solvent type and density. Moreover, both the squeezing and combustion methods can be adopted for reusing the graphene aerogels. Finally, the graphene aerogels exhibit stable and sensitive current responses, making them the ideal candidates for applications as multifunctional pressure/strain sensors such as wearable devices.     

Wearable,Human‐Interactive,Health‐Monitoring,Wireless Devices Fabricated by Macroscale Printing Techniques

Wearable human‐interactive devices are advanced technologies that will improve the comfort, convenience, and security of humans, and have a wide range of applications from robotics to clinical health monitoring. In this study, a fully printed wearable human‐interactive device called a “smart bandage” is proposed as the first proof of concept. The device incorporates touch and temperature sensors to monitor health, a drug‐delivery system to improve health, and a wireless coil to detect touch. The sensors, microelectromechanical systems (MEMS) structure, and wireless coil are monolithically integrated onto flexible substrates. A smart bandage is demonstrated on a human arm. These types of wearable human‐interactive devices represent a promising platform not only for interactive devices, but also for flexible MEMS technology.     

Large‐Area Compliant,Low‐Cost,and Versatile Pressure‐Sensing Platform Based on Microcrack‐Designed Carbon Black@Polyurethane Sponge for Human–Machine Interfacing

It is a challenge to manufacture pressure‐sensing materials that possess flexibility, high sensitivity, large‐area compliance, and capability to detect both tiny and large motions for the development of artificial intelligence products. Herein, a very simple and low‐cost approach is proposed to fabricate versatile pressure sensors based on microcrack‐designed carbon black (CB)@polyurethane (PU) sponges via natural polymer‐mediated water‐based layer‐by‐layer assembly. These sensors are capable of satisfying the requirements of ultrasmall as well as large motion monitoring. The versatility of these sensors benefits from two aspects: microcrack junction sensing mechanism for tiny motion detecting (91 Pa pressure, 0.2% strain) inspired by the spider sensory system and compressive contact of CB@PU conductive backbones for large motion monitoring (16.4 kPa pressure, 60% strain). Furthermore, these sensors exhibit excellent flexibility, fast response times (<20 ms), as well as good reproducibility over 50 000 cycles. This study also demonstrates the versatility of these sensors for various applications, ranging from speech recognition, health monitoring, bodily motion detection to artificial electronic skin. The desirable comprehensive performance of our sensors, which is comparable to the recently reported pressure‐sensing devices, together with their significant advantages of low‐cost, easy fabrication, especially versatility, makes them attractive in the future of artificial intelligence.     

Highly Sensitive,Wearable, Durable Strain Sensors and Stretchable Conductors Using Graphene/Silicon Rubber Composites

Highly sensitive, wearable and durable strain sensors are vital to the development of health monitoring systems, smart robots and human machine interfaces. The recent sensor fabrication progress is respectable, but it is limited by complexity, low sensitivity and unideal service life. Herein a facile, cost‐effective and scalable method is presented for the development of high‐performance strain sensors and stretchable conductors based on a composite film consisting of graphene platelets (GnPs) and silicon rubber. Through calculation by the tunneling theory using experimental data, the composite film has demonstrated ideal linear and reproducible sensitivity to tensile strains, which is contributed by the superior piezoresistivity of GnPs having tunable gauge factors 27.7–164.5. The composite sensors fabricated in different days demonstrate pretty similar performance, enabling applications as a health‐monitoring device to detect various human motions from finger bending to pulse. They can be used as electronic skin, a vibration sensor and a human‐machine interface controller. Stretchable conductors are made by coating and encapsulating GnPs with polydimethyl siloxane to create another composite; this structure allows the conductor to be readily bent and stretched with sufficient mechanical robustness and cyclability.     

Recent Advances in Sensing Applications of Graphene Assemblies and Their Composites

Development of next‐generation sensor devices is gaining tremendous attention in both academia and industry because of their broad applications in manufacturing processes, food and environment control, medicine, disease diagnostics, security and defense, aerospace, and so forth. Current challenges include the development of low‐cost, ultrahigh, and user‐friendly sensors, which have high selectivity, fast response and recovery times, and small dimensions. The critical demands of these new sensors are typically associated with advanced nanoscale sensing materials. Among them, graphene and its derivatives have demonstrated the ideal properties to overcome these challenges and have merged as one of the most popular sensing platforms for diverse applications. A broad range of graphene assemblies with different architectures, morphologies, and scales (from nano‐, micro‐, to macrosize) have been explored in recent years for designing new high‐performing sensing devices. Herein, this study presents and discusses recent advances in synthesis strategies of assembled graphene‐based superstructures of 1D, 2D, and 3D macroscopic shapes in the forms of fibers, thin films, and foams/aerogels. The fabricated state‐of‐the‐art applications of these materials in gas and vapor, biomedical, piezoresistive strain and pressure, heavy metal ion, and temperature sensors are also systematically reviewed and discussed, and their sensing performance is compared.     

MXene‐Reinforced Cellulose Nanofibril Inks for 3D‐Printed Smart Fibres and Textiles

Fibre‐based materials have received tremendous attention due to their flexibility and wearability. Although great efforts have been devoted to achieve high‐performance fibres over the past several years, it is still challenging for multifunctional macroscopic fibres to satisfy versatile applications. 2D transition metal carbides/nitrides (MXenes) with intriguing physical/chemical properties have been explored in broad application, and may be able to reinforce synthetic fibres. Inspired by natural materials, for the first time, flexible smart fibres and textiles are fabricated using a 3D printing process with hybrid inks of TEMPO (2,2,6,6‐tetramethylpiperidine‐1‐oxylradi‐cal)‐mediated oxidized cellulose nanofibrils (TOCNFs) and Ti₃C₂ MXene. The hybrid inks display good rheological properties, which allow them to achieve accurate structures and be rapidly printed. TOCNFs/Ti₃C₂ in hybrid inks self‐assemble to fibres with an aligned structure in ethanol, mimicking the features of the natural structures of plant fibres. In contrast to conventional synthetic fibres with limited functions, smart TOCNFs/Ti₃C₂ fibres and textiles exhibit significant responsiveness to multiple external stimuli (electrical/photonic/mechanical). TOCNFs/Ti₃C₂ textiles with electromechanical performance can be processed into sensitive strain sensors. Such multifunctional smart fibres and textiles will be promising in diverse applications, including wearable heating textiles, human health monitoring, and human–machine interfaces.