Plasticizing Silk Protein for On‐Skin Stretchable Electrodes

Soft and stretchable electronic devices are important in wearable and implantable applications because of the high skin conformability. Due to the natural biocompatibility and biodegradability, silk protein is one of the ideal platforms for wearable electronic devices. However, the realization of skin‐conformable electronic devices based on silk has been limited by the mechanical mismatch with skin, and the difficulty in integrating stretchable electronics. Here, silk protein is used as the substrate for soft and stretchable on‐skin electronics. The original high Young's modulus (5–12 GPa) and low stretchability (<20%) are tuned into 0.1–2 MPa and > 400%, respectively. This plasticization is realized by the addition of CaCl₂ and ambient hydration, whose mechanism is further investigated by molecular dynamics simulations. Moreover, highly stretchable (>100%) electrodes are obtained by the thin‐film metallization and the formation of wrinkled structures after ambient hydration. Finally, the plasticized silk electrodes, with the high electrical performance and skin conformability, achieve on‐skin electrophysiological recording comparable to that by commercial gel electrodes. The proposed skin‐conformable electronics based on biomaterials will pave the way for the harmonized integration of electronics into human.     

Ultrastretchable Conductor Fabricated on Skin‐Like Hydrogel–Elastomer Hybrid Substrates for Skin Electronics

Printing technology can be used for manufacturing stretchable electrodes, which represent essential parts of wearable devices requiring relatively high degrees of stretchability and conductivity. In this work, a strategy for fabricating printable and highly stretchable conductors are proposed by transferring printed Ag ink onto stretchable substrates comprising Ecoflex elastomer and tough hydrogel layers using a water‐soluble tape. The elastic modulus of the produced hybrid film is close to that of the hydrogel layer, since the thickness of Ecoflex elastomer film coated on hydrogel is very thin (30 µm). Moreover, the fabricated conductor on hybrid film is stretched up to 1780% strain. The described transfer method is simpler than other techniques utilizing elastomer stamps or sacrificial layers and enables application of printable electronics to the substrates with low elastic moduli (such as hydrogels). The integration of printed electronics with skin‐like low‐modulus substrates can be applied to make wearable devices more comfortable for human skin.     

Tough and Water‐Insensitive Self‐Healing Elastomer for Robust Electronic Skin

An electronic (e‐) skin is expected to experience significant wear and tear over time. Therefore, self‐healing stretchable materials that are simultaneously soft and with high fracture energy, that is high tolerance of damage or small cracks without propagating, are essential requirements for the realization of robust e‐skin. However, previously reported elastomers and especially self‐healing polymers are mostly viscoelastic and lack high mechanical toughness. Here, a new class of polymeric material crosslinked through rationally designed multistrength hydrogen bonding interactions is reported. The resultant supramolecular network in polymer film realizes exceptional mechanical properties such as notch‐insensitive high stretchability (1200%), high toughness of 12 000 J m^?2, and autonomous self‐healing even in artificial sweat. The tough self‐healing materials enable the wafer‐scale fabrication of robust and stretchable self‐healing e‐skin devices, which will provide new directions for future soft robotics and skin prosthetics.     

Fully Integrated Design of a Stretchable Solid‐State Lithium‐Ion Full Battery

A solid‐state lithium‐ion battery, in which all components (current collector, anode and cathode, electrolyte, and packaging) are stretchable, is introduced, giving rise to a battery design with mechanical properties that are compliant with flexible electronic devices and elastic wearable systems. By depositing Ag microflakes as a conductive layer on a stretchable carbon–polymer composite, a current collector with a low sheet resistance of ≈2.7 Ω □^?1 at 100% strain is obtained. Stretchable electrodes are fabricated by integrating active materials with the elastic current collector. A polyacrylamide–“water‐in‐salt” electrolyte is developed, offering high ionic conductivity of 10^?3 to 10^?2 S cm^?1 at room temperature and outstanding stretchability up to ≈300% of its original length. Finally, all these components are assembled into a solid‐state lithium‐ion full cell in thin‐film configuration. Thanks to the deformable individual components, the full cell functions when stretched, bent, or even twisted. For example, after stretching the battery to 50%, a reversible capacity of 28 mAh g^?1 and an average energy density of 20 Wh kg^?1 can still be obtained after 50 cycles at 120 mA g^?1, confirming the functionality of the battery under extreme mechanical stress.     

3D‐Structured Stretchable Strain Sensors for Out‐of‐Plane Force Detection

Stretchable strain sensors, as the soft mechanical interface, provide the key mechanical information of the systems for healthcare monitoring, rehabilitation assistance, soft exoskeletal devices, and soft robotics. Stretchable strain sensors based on 2D flat film have been widely developed to monitor the in‐plane force applied within the plane where the sensor is placed. However, to comprehensively obtain the mechanical feedback, the capability to detect the out‐of‐plane force, caused by the interaction outside of the plane where the senor is located, is needed. Herein, a 3D‐structured stretchable strain sensor is reported to monitor the out‐of‐plane force by employing 3D printing in conjunction with out‐of‐plane capillary force‐assisted self‐pinning of carbon nanotubes. The 3D‐structured sensor possesses large stretchability, multistrain detection, and strain‐direction recognition by one single sensor. It is demonstrated that out‐of‐plane forces induced by the air/fluid flow are reliably monitored and intricate flow details are clearly recorded. The development opens up for the exploration of next‐generation 3D stretchable sensors for electronic skin and soft robotics.     

An All‐Stretchable‐Component Sodium‐Ion Full Battery

Stretchable energy‐storage devices receive considerable attention due to their promising applications in future wearable technologies. However, they currently suffer from many problems, including low utility of active materials, limited multidirectional stretchability, and poor stability under stretched conditions. In addition, most proposed designs use one or more rigid components that fail to meet the stretchability requirement for the entire device. Here, an all‐stretchable‐component sodium‐ion full battery based on graphene‐modified poly(dimethylsiloxane) sponge electrodes and an elastic gel membrane is developed for the first time. The battery exhibits reasonable electrochemical performance and robust mechanical deformability; its electrochemical characteristics can be well‐maintained under many different stretched conditions and after hundreds of stretching–release cycles. This novel design integrating all stretchable components provides a pathway toward the next generation of wearable energy devices in modern electronics.     

Highly Stable and Stretchable Conductive Films through Thermal‐Radiation‐Assisted Metal Encapsulation

Stretchable conductors are the basic units of advanced flexible electronic devices, such as skin‐like sensors, stretchable batteries and soft actuators. Current fabrication strategies are mainly focused on the stretchability of the conductor with less emphasis on the huge mismatch of the conductive material and polymeric substrate, which results in stability issues during long‐term use. Thermal‐radiation‐assisted metal encapsulation is reported to construct an interlocking layer between polydimethylsiloxane (PDMS) and gold by employing a semipolymerized PDMS substrate to encapsulate the gold clusters/atoms during thermal deposition. The stability of the stretchable conductor is significantly enhanced based on the interlocking effect of metal and polymer, with high interfacial adhesion (>2 MPa) and cyclic stability (>10 000 cycles). Also, the conductor exhibits superior properties such as high stretchability (>130%) and large active surface area (>5:1 effective surface area/geometrical area). It is noted that this method can be easily used to fabricate such a stretchable conductor in a wafer‐scale format through a one‐step process. As a proof of concept, both long‐term implantation in an animal model to monitor intramuscular electric signals and on human skin for detection of biosignals are demonstrated. This design approach brings about a new perspective on the exploration of stretchable conductors for biomedical applications.     

Crumpling and Unfolding of Montmorillonite Hybrid Nanocoatings as Stretchable Flame‐Retardant Skin

Flame‐retardant coatings are widely used in a variety of personnel or product protection, and many applications would benefit from film stretchability if suitable materials are available. It is challenging to develop flame‐retardant coatings that are stretchable, eco‐friendly, and capable of being integrated on mechanically dynamic devices. Here, a concept is reported that uses pretextured montmorillonite (MMT) hybrid nanocoatings that can undergo programed unfolding to mimic the stretchability of elastomeric materials. These textured MMT coatings can be transferred onto an elastomeric substrate to achieve an MMT/elastomer bilayer device with high stretchability (225% areal strain) and effective flame retardancy. The bilayer composite is utilized as flame‐retardant skin for a soft robotic gripper, and it is demonstrated that the actuated response can manipulate and rescue irregularly shaped objects from a fire scene. Furthermore, by depositing the conformal MMT nanocoatings on nitrile gloves, the firefree gloves can endure direct flame contact without ignition.     

Ultraflexible Near‐Infrared Organic Photodetectors for Conformal Photoplethysmogram Sensors

Flexible organic optoelectronic devices simultaneously targeting mechanical conformability and fast responsivity in the near‐infrared (IR) region are a prerequisite to expand the capabilities of practical optical science and engineering for on‐skin optoelectronic applications. Here, an ultraflexible near‐IR responsive skin‐conformal photoplethysmogram sensor based on a bulk heterojunction photovoltaic active layer containing regioregular polyindacenodithiophene‐pyridyl[2,1,3]thiadiazole‐cyclopentadithiophene (PIPCP) is reported. The ultrathin (3 µm thick) photodetector exhibits unprecedented operational stability under severe mechanical deformation at a bending radius of less than 3 µm, even after more than 10³ bending cycles. Deliberate optimization of the physical dimensions of the active layer used in the device enables precise on/off switching and high device yield simultaneously. The response frequency over 1 kHz under mechanically deformed conditions facilitates conformal electronic sensors at the machine/human interface. Finally, a mechanically stretchable, flexible, and skin‐conformal photoplethysmogram (PPG) device with higher sensitivity than those of rigid devices is demonstrated, through conformal adherence to the flexuous surface of a fingerprint.     

Transparent,stretchable, and rapid-response humidity sensor for body-attachable wearable electronics

Stretchable and conformal humidity sensors that can be attached to the human body for continuously monitoring the humidity of the environment around the human body or the moisture level of the human skin can play an important role in electronic skin and personal healthcare applications.However,most stretchable humidity sensors are based on the geometric engineering of non-stretchable components and only a few detailed studies are available on stretchable humidity sensors under applied mechanical deformations.In this paper,we propose a transparent,stretchable humidity sensor with a simple fabrication process,having intrinsically stretchable components that provide high stretchability,sensitivity,and stability along with fast response and relaxation time.Composed of reduced graphene oxide-polyurethane composites and an elastomeric conductive electrode,this device exhibits impressive response and relaxation time as fast as 3.5 and 7 s,respectively.The responsivity and the response and relaxation time of the device in the presence of humidity remain almost unchanged under stretching up to a strain of 60％ and after 10,000 stretching cycles at a 40％ strain.Further,these stretchable humidity sensors can be easily and conformally attached to a finger for monitoring the humidity levels of the environment around the human body,wet objects,or human skin.     

Advances in Rational Design and Materials of High‐Performance Stretchable Electromechanical Sensors

Stretchable and wearable sensor technology has attracted significant interests and created high technological impact on portable healthcare and smart human–machine interfaces. Wearable electromechanical systems are an important part of this technology that has recently witnessed tremendous progress toward high‐performance devices for commercialization. Over the past few years, great attention has been paid to simultaneously enhance the sensitivity and stretchability of the electromechanical sensors toward high sensitivity, ultra‐stretchability, low power consumption or self‐power functionalities, miniaturisation as well as simplicity in design and fabrication. This work presents state‐of‐the‐art advanced materials and rational designs of electromechanical sensors for wearable applications. Advances in various sensing concepts and structural designs for intrinsic stretchable conductive materials as well as advanced rational platforms are discussed. In addition, the practical applications and challenges in the development of stretchable electromechanical sensors are briefly mentioned and highlighted.     

Stretchable Electronic Sensors of Nanocomposite Network Films for Ultrasensitive Chemical Vapor Sensing

A stretchable, transparent, and body‐attachable chemical sensor is assembled from the stretchable nanocomposite network film for ultrasensitive chemical vapor sensing. The stretchable nanocomposite network film is fabricated by in situ preparation of polyaniline/MoS₂ (PANI/MoS₂) nanocomposite in MoS₂ suspension and simultaneously nanocomposite deposition onto prestrain elastomeric polydimethylsiloxane substrate. The assembled stretchable electronic sensor demonstrates ultrasensitive sensing performance as low as 50 ppb, robust sensing stability, and reliable stretchability for high‐performance chemical vapor sensing. The ultrasensitive sensing performance of the stretchable electronic sensors could be ascribed to the synergistic sensing advantages of MoS₂ and PANI, higher specific surface area, the reliable sensing channels of interconnected network, and the effectively exposed sensing materials. It is expected to hold great promise for assembling various flexible stretchable chemical vapor sensors with ultrasensitive sensing performance, superior sensing stability, reliable stretchability, and robust portability to be potentially integrated into wearable electronics for real‐time monitoring of environment safety and human healthcare.     

A Stretchable and Self‐Healing Energy Storage Device Based on Mechanically and Electrically Restorative Liquid‐Metal Particles and Carboxylated Polyurethane Composites

Stretchable and self‐healing (SH) energy storage devices are indispensable elements in energy‐autonomous electronic skin. However, the current collectors are not self‐healable nor intrinsically stretchable, they mostly rely on strain‐accommodating structures that require complex processing, are often limited in stretchability, and suffer from low device packing density and fragility. Here, an SH conductor comprising nickel flakes, eutectic gallium indium particles (EGaInPs), and carboxylated polyurethane (CPU) is presented. An energy storage device is constructed by the two SH electrodes assembled with graphene nanoplatelets sandwiching an ionic‐liquid electrolyte. An excellent electrochemical healability (94% capacity retention upon restretching at 100% after healing from bifurcation) is unveiled, stemming from the complexation modulated redox behavior of EGaIn in the presence of the ligand bis(trifluoromethanesulfonyl)imide, which enhances the reversible Faradaic reaction of Ga. Self‐healing can be achieved where the damaged regions are electrically restored by the flow of liquid metal and mechanically healing activated by the interfacial hydrogen bonding of CPU with an efficiency of 97.5% can be achieved. The SH conductor has an initial conductivity of 2479 S cm^?1 that attains a high stretchability with 700% strain, it restores 100% stretchability even after breaking/healing with the electrical healing efficiency of 75%.     

On‐Skin Triboelectric Nanogenerator and Self‐Powered Sensor with Ultrathin Thickness and High Stretchability

Researchers have devoted a lot of efforts on pursuing light weight and high flexibility for the wearable electronics, which also requires the related energy harvesting devices to have ultrathin thickness and high stretchability. Hence, an elastic triboelectric nanogenerator (TENG) is proposed that can serve as the second skin on human body. The total thickness of this TENG is about 102 µm and the device can work durably under a strain of 100%. The carbon grease is painted on the surface of elastomer film to work as stretchable electrode and thus the fine geometry control of the electrode can be achieved. This elastic TENG can even work on the human fingers without disturbing body movement. The open‐circuit voltage and short‐circuit current from the device with a contact area of 9 cm² can reach 115 V and 3 µA, respectively. Two kinds of self‐powered sensor systems with optimized identification strategies are also designed to demonstrate the application possibility of this elastic TENG. The superior characteristics of ultrathin thickness, high stretchability, and fine geometry control of this TENG can promote many potential applications in the field of wearable self‐powered sensory system, electronics skin, artificial muscles, and soft robotics.     

Fabrication of Flexible MoS2 Thin‐Film Transistor Arrays for Practical Gas‐Sensing Applications

By combining two kinds of solution‐processable two‐dimensional materials, a flexible transistor array is fabricated in which MoS₂ thin film is used as the active channel and reduced graphene oxide (rGO) film is used as the drain and source electrodes. The simple device configuration and the 1.5 mm‐long MoS₂ channel ensure highly reproducible device fabrication and operation. This flexible transistor array can be used as a highly sensitive gas sensor with excellent reproducibility. Compared to using rGO thin film as the active channel, this new gas sensor exhibits much higher sensitivity. Moreover, functionalization of the MoS₂ thin film with Pt nanoparticles further increases the sensitivity by up to ～3 times. The successful incorporation of a MoS₂ thin‐film into the electronic sensor promises its potential application in various electronic devices.     

A Solution‐Processable,Omnidirectionally Stretchable,and High‐Pressure‐Sensitive Piezoresistive Device

The development of omnidirectionally stretchable pressure sensors with high performance without stretching‐induced interference has been hampered by many challenges. Herein, an omnidirectionally stretchable piezoresistive pressure‐sensing device is demonstrated by combining an omniaxially stretchable substrate with a 3D micropattern array and solution‐printing of electrode and piezoresistive materials. A unique substrate structural design and materials mean that devices that are highly sensitive are rendered, with a stable out‐of‐plane pressure response to both static (sensitivity of 0.5 kPa^?1 and limit of detection of 28 Pa) and dynamic pressures and the minimized in‐plane stretching responsiveness (a small strain gauge factor of 0.17), achieved through efficient strain absorption of the electrode and sensing materials. The device can detect human‐body tremors, as well as measure the relative elastic properties of human skin. The omnidirectionally stretchable pressure sensor with a high pressure sensitivity and minimal stretch‐responsiveness yields great potential to skin‐attachable wearable electronics, human–machine interfaces, and soft robotics applications.     

Pencil‐Drawing Skin‐Mountable Micro‐Supercapacitors

In this study, integrated plaster‐like micro‐supercapacitors based on medical adhesive tapes are fabricated by a simple pencil drawing process combined with a mild solution deposition of MnO₂. These solid micro‐supercapacitors not only exhibit excellent stretchability, flexibility, and biocompatibility, but also possess outstanding electrochemical performances, such as exceptional rate capability and cycling stability. Hence they may act as skin‐mountable and thin‐film energy storage devices of high efficiency to power miniaturized and wearable electronic devices.     

Graphene‐Coated Spandex Sensors Embedded into Silicone Sheath for Composites Health Monitoring and Wearable Applications

This study presents a low‐cost, tunable, and stretchable sensor fabricated based on spandex (SpX) yarns coated with graphene nanoplatelets (GnP) through a dip‐coating process. The SpX/GnP is wrapped into a stretchable silicone rubber (SR) sheath to protect the conductive layer against harsh conditions, which allows for fabricating washable wearable sensors. Dip‐coating parameters are optimized to obtain the maximum GnP coating rate. The covering sheath is tailored to achieve high stretchability beyond the sensing limit of 104% for SpX/GnP/SR sensors. Adjustable sensitivity is attained by manipulating SpX immersion times broadening its application for a wide range of strains: Gauge factors as high as two orders of magnitude are achieved at tensile strains greater than ≈40%. The fabricated sensors are tested for two applications: First, the SpX/GnP sensors are integrated into composite fabrics (with no negative impact on the structural integrity of the part) for screening the yarn displacements, resin flow, solidification during the hot press forming process, and structural health monitoring under mechanical loads with minimal cross‐sensitivity to temperature/humidity. Second, the capability of SpX/GnP/SP sensors in detection of a wide range of bodily motions (from the joint motion to arterial blood pressure) is demonstrated.     

Wetting‐Induced Climbing for Transferring Interfacially Assembled Large‐Area Ultrathin Pristine Graphene Film

Owing to inherent 2D structure, marvelous mechanical, electrical, and thermal properties, graphene has great potential as a macroscopic thin film for surface coating, composite, flexible electrode, and sensor. Nevertheless, the production of large‐area graphene‐based thin film from pristine graphene dispersion is severely impeded by its poor solution processability. In this study, a robust wetting‐induced climbing strategy is reported for transferring the interfacially assembled large‐area ultrathin pristine graphene film. This strategy can quickly convert solvent‐exfoliated pristine graphene dispersion into ultrathin graphene film on various substrates with different materials (glass, metal, plastics, and cloth), shapes (film, fiber, and bulk), and hydrophobic/hydrophilic patterns. It is also applicable to nanoparticles, nanofibers, and other exfoliated 2D nanomaterials for fabricating large‐area ultrathin films. Alternate climbing of different ultrathin nanomaterial films allows a layer‐by‐layer transfer, forming a well‐ordered layered composite film with the integration of multiple pristine nanomaterials at nanometer scale. This powerful strategy would greatly promote the development of solvent‐exfoliated pristine nanomaterials from dispersions to macroscopic thin film materials.     

Flexible,Stretchable, and Transparent Planar Microsupercapacitors Based on 3D Porous Laser‐Induced Graphene

The graphene with 3D porous network structure is directly laser‐induced on polyimide sheets at room temperature in ambient environment by an inexpensive and one‐step method, then transferred to silicon rubber substrate to obtain highly stretchable, transparent, and flexible electrode of the all‐solid‐state planar microsupercapacitors. The electrochemical capacitance properties of the graphene electrodes are further enhanced by nitrogen doping and with conductive poly(3,4‐ethylenedioxythiophene) coating. With excellent flexibility, stretchability, and capacitance properties, the planar microsupercapacitors present a great potential in fashionable and comfortable designs for wearable electronics.