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.     

Local Crack‐Programmed Gold Nanowire Electronic Skin Tattoos for In‐Plane Multisensor Integration

Sensitive, specific, yet multifunctional tattoo‐like electronics are ideal wearable systems for “any time, any where” health monitoring because they can virtually become parts of the human skin, offering a burdenless “unfeelable” wearing experience. A skin‐like, multifunctional electronic tattoo made entirely from gold using a standing enokitake‐mushroom‐like vertically aligned nanowire membrane in conjunction with a programmable local cracking technology is reported. Unlike previous multifunctional systems, only a single material type is needed for the integrated gold circuits involved in interconnects and multiplexed specific sensors, thereby avoiding the use of complex multimaterials interfaces. This is possiblebecause the programmable local cracking technology allows for the arbitrary fine‐tuning of the properties of elastic gold conductors from strain‐insensitive to highly strain‐sensitive simply by adjusting localized crack size, shape, and orientations—a capability impossible to achieve with previous bulk cracking technology. Furthermore, in‐plane integration of strain/pressure sensors, anisotropic orientation‐specific sensors, strain‐insensitive stretchable interconnects, temperature sensors, glucose sensors, and lactate sensors without the need of soldering or gluing are demonstrated. This strategy opens a new general route for the design of next‐generation wearable electronic tattoos.     

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.     

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.     

Microtopography‐Guided Conductive Patterns of Liquid‐Driven Graphene Nanoplatelet Networks for Stretchable and Skin‐Conformal Sensor Array

Flexible thin‐film sensors have been developed for practical uses in invasive or noninvasive cost‐effective healthcare devices, which requires high sensitivity, stretchability, biocompatibility, skin/organ‐conformity, and often transparency. Graphene nanoplatelets can be spontaneously assembled into transparent and conductive ultrathin coatings on micropatterned surfaces or planar substrates via a convective Marangoni force in a highly controlled manner. Based on this versatile graphene assembled film preparation, a thin, stretchable and skin‐conformal sensor array (144 pixels) is fabricated having microtopography‐guided, graphene‐based, conductive patterns embedded without any complicated processes. The electrically controlled sensor array for mapping spatial distributions (144 pixels) shows high sensitivity (maximum gauge factor ≈1697), skin‐like stretchability (<48%), high cyclic stability or durability (over 10⁵ cycles), and the signal amplification (≈5.25 times) via structure‐assisted intimate‐contacts between the device and rough skin. Furthermore, given the thin‐film programmable architecture and mechanical deformability of the sensor, a human skin‐conformal sensor is demonstrated with a wireless transmitter for expeditious diagnosis of cardiovascular and cardiac illnesses, which is capable of monitoring various amplified pulse‐waveforms and evolved into a mechanical/thermal‐sensitive electric rubber‐balloon and an electronic blood‐vessel. The microtopography‐guided and self‐assembled conductive patterns offer highly promising methodology and tool for next‐generation biomedical devices and various flexible/stretchable (wearable) devices.     

Stretchable Organometal‐Halide‐Perovskite Quantum‐Dot Light‐Emitting Diodes

Stretchable light‐emitting diodes (LEDs) and electroluminescent capacitors have been reported to potentially bring new opportunities to wearable electronics; however, these devices lack in efficiency and/or stretchability. Here, a stretchable organometal‐halide‐perovskite quantum‐dot LED with both high efficiency and mechanical compliancy is demonstrated. The hybrid device employs an ultrathin (<3 µm) LED structure conformed on a surface‐wrinkled elastomer substrate. Its luminescent efficiency is up to 9.2 cd A^?1, which is 70% higher than a control diode fabricated on the rigid indium tin oxide/glass substrate. Mechanical deformations up to 50% tensile strain do not induce significant loss of the electroluminescent property. The device can survive 1000 stretch–release cycles of 20% tensile strain with small fluctuations in electroluminescent performance.     

Silver‐Quantum‐Dot‐Modified MoO3 and MnO2 Paper‐Like Freestanding Films for Flexible Solid‐State Asymmetric Supercapacitors

Free‐standing paper‐like thin‐film electrodes have great potential to boost next‐generation power sources with highly flexible, ultrathin, and lightweight requirements. In this work, silver‐quantum‐dot‐ (2–5 nm) modified transition metal oxide (including MoO₃ and MnO₂) paper‐like electrodes are developed for energy storage applications. Benefitting from the ohmic contact at the interfaces between silver quantum dots and MoO₃ nanobelts (or MnO₂ nanowires) and the binder‐free nature and 0D/1D/2D nanostructured 3D network of the fabricated electrodes, substantial improvements on the electrical conductivity, efficient ionic diffusion, and areal capacitances of the hybrid nanostructure electrodes are observed. With this proposed strategy, the constructed asymmetric supercapacitors, with Ag quantum dots/MoO₃ “paper” as anode, Ag quantum dots/MnO₂ “paper” as cathode, and neutral Na₂SO₄/polyvinyl alcohol hydrogel as electrolyte, exhibit significantly enhanced energy and power densities in comparison with those of the supercapacitors without modification of Ag quantum dots on electrodes; present excellent cycling stability at different current densities and good flexibility under various bending states; offer possibilities as high‐performance power sources with low cost, high safety, and environmental friendly properties.     

Cryo‐Transferred Ultrathin and Stretchable Epidermal Electrodes

A simple cryo‐transfer method to fabricate ultrathin, stretchable, and conformal epidermal electrodes based on a combination of silver nanowires (AgNWs) network and elastomeric polymers is developed. This method can temporarily enable the soft elastomers with much higher elastic modulus and dimensional contraction through exploiting their glass‐transition behaviors. During this process, a much higher Von Mises stress can be loaded on AgNWs than usual, and the generated strong grip force can facilitate the complete transfer of AgNWs. Afterward, the thawed AgNWs and elastomer composites quickly recover to their soft state at room temperature. The obtained ultrathin and soft electrode with a thickness of 8.4 µm and transmittance of 90.8% at a sheet resistance of 13.2 Ω sq^?1 can tolerate a stretching strain of 70% and 50 000 repeated bending cycles, which meets rigorous requirements of epidermal applications. The as‐prepared epidermal electrodes are effective and comfortable for electrophysiological signal monitoring, and while showing excellent performance exceeding the commercialized gel electrodes.     

A High Aspect Ratio Serpentine Structure for Use As a Strain‐Insensitive,Stretchable Transparent Conductor

The development of strain‐insensitive stretchable transparent conductors (TCs) is essential for manufacturing stretchable electronics. Despite recent progress, achieving a high optoelectronic performance under applied strain of 50% continues to present a significant challenge in this research field. Herein, an ultratall and ultrathin high aspect ratio serpentine metal structure is described that exhibits a remarkable stretching ability (the resistance remains constant under applied strain of 100%) and simultaneously provides an excellent transparent conducting performance (with a sheet resistance of 7.6 Ω ^?1 and a transmittance of 90.5%). It is demonstrated that the highly stretchable transparent conducting properties can be attributed to the high aspect ratio feature. A high aspect ratio (aspect ratio of 17–367) structure permits facile deformation of the serpentine structure with in‐plane motion, leading to a high stretching ability. In addition, this structural feature avoids the classic tradeoff between optical transmittance and electrical conductance, providing a high electrical conductance without decreasing the optical transmittance. The practical utility of these devices is tested by using these TCs as stretchable interconnectors among LEDs or in wearable VOC gas sensors.     

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.     

Editable Supercapacitors with Customizable Stretchability Based on Mechanically Strengthened Ultralong MnO2 Nanowire Composite

Although some progress has been made on stretchable supercapacitors, traditional stretchable supercapacitors fabricated by predesigning structured electrodes for device assembling still lack the device‐level editability and programmability. To adapt to wearable electronics with arbitrary configurations, it is highly desirable to develop editable supercapacitors that can be directly transferred into desirable shapes and stretchability. In this work, editable supercapacitors for customizable shapes and stretchability using electrodes based on mechanically strengthened ultralong MnO₂ nanowire composites are developed. A supercapacitor edited with honeycomb‐like structure shows a specific capacitance of 227.2 mF cm^?2 and can be stretched up to 500% without degradation of electrochemical performance, which is superior to most of the state‐of‐the‐art stretchable supercapacitors. In addition, it maintains nearly 98% of the initial capacitance after 10 000 stretch‐and‐release cycles under 400% tensile strain. As a representative of concept for system integration, the editable supercapacitors are integrated with a strain sensor, and the system exhibits a stable sensing performance even under arm swing. Being highly stretchable, easily programmable, as well as connectable in series and parallel, an editable supercapacitor with customizable stretchability is promising to produce stylish energy storage devices to power various portable, stretchable, and wearable devices.     

Design of Novel Wearable,Stretchable, and Waterproof Cable‐Type Supercapacitors Based on High‐Performance Nickel Cobalt Sulfide‐Coated Etching‐Annealed Yarn Electrodes

Rapid advances in functional electronics bring tremendous demands on innovation toward effective designs of device structures. Yarn supercapacitors (SCs) show advantages of flexibility, knittability, and small size, and can be integrated into various electronic devices with low cost and high efficiency for energy storage. In this work, functionalized stainless steel yarns are developed to support active materials of positive and negative electrodes, which not only enhance capacitance of both electrodes but can also be designed into stretchable configurations. The as‐made asymmetric yarn SCs show a high energy density of 0.0487 mWh cm^?2 (10.19 mWh cm^?3) at a power density of 0.553 mW cm^?2 (129.1 mW cm^?3) and a specific capacitance of 127.2 mF cm^?2 under an operating voltage window of 1.7 V. The fabricated SC is then made into a stretchable configuration by a prestraining‐then‐releasing approach using polydimethylsiloxane (PDMS) tube, and its electrochemical performance can be well maintained when stretching up to a high strain of 100%. Moreover, the stretchable cable‐type SCs are stably workable under water‐immersed condition. The method opens up new ways for fabricating flexible, stretchable, and waterproof devices.     

Nitrogen‐Doped Carbon Encapsulated Mesoporous Vanadium Nitride Nanowires as Self‐Supported Electrodes for Flexible All‐Solid‐State Supercapacitors

Flexible 3D nanoarchitectures have received tremendous interest recently because of their potential applications in flexible/wearable energy storage devices. Herein, 3D intertwined nitrogen‐doped carbon encapsulated mesoporous vanadium nitride nanowires (MVN@NC NWs) are investigated as thin, lightweight, and self‐supported electrodes for flexible supercapacitors (SCs). The MVN NWs have abundant active sites accessible to charge storage, and the N‐doped carbon shell suppresses electrochemical dissolution of the inner MVN NWs in an alkaline electrolyte, leading to excellent capacitive properties. The flexible MVN@NC NWs film electrode delivers a high areal capacitance of 282 mF cm⁻² and exhibits excellent long‐term stability with 91.8% capacitance retention after 12 000 cycles in a KOH electrolyte. All‐solid‐state flexible SCs assembled by sandwiching two flexible MVN@NC NWs film electrodes with alkaline poly(vinyl alcohol) (PVA), sodium polyacrylate, and KOH gel electrolyte boast a high volumetric capacitance of 10.9 F cm⁻³, an energy density of 0.97 mWh cm⁻³, and a power density of 2.72 W cm⁻³ at a current density of 0.051 A cm⁻³ based on the entire cell. By virtue of the excellent mechanical flexibility, high capacitance, and large energy/power density, the self‐supported MVN@NC NWs paper‐like electrodes have large potential applications in portable and wearable flexible electronics.     

Metal Deposition on a Self‐Generated Microfibril Network to Fabricate Stretchable Tactile Sensors Providing Analog Position Information

Stretchable conductors and sensors have attracted great attention for use in electronic skin and healthcare monitoring. Despite the development of many stretchable conductors, there are still very few studies that utilize the conventional methods making electrodes and circuits used in current industry. A method is proposed to fabricate a stretchable electrode pattern and a stretchable tactile sensor by simply depositing linear metal lines through a mask on a stretchable substrate. A method is developed of a self‐generating microfibril network on the surface of stretchable block copolymer substrates. The formation mechanism of the microfibril network is studied with finite element method simulations. Metals (Au and Ag nanowires) are deposited directly on the substrate through a patterned mask. This study shows that strain‐insensitive circuit and strain‐sensitive sensor can be fabricated in a controlled way by adjusting the thickness of the deposited metal, which makes it easy to fabricate a tactile sensor by metal deposition. Also, by using the characteristic that the sensor has different sensitivity depending on the line pattern width, a novel sensor structure simultaneously providing analog‐type position information and pressure value is proposed.     

Ultrahigh‐Energy Density Lithium‐Ion Cable Battery Based on the Carbon‐Nanotube Woven Macrofilms

Moore's law predicts the performance of integrated circuit doubles every two years, lasting for more than five decades. However, the improvements of the performance of energy density in batteries lag far behind that. In addition, the poor flexibility, insufficient‐energy density, and complexity of incorporation into wearable electronics remain considerable challenges for current battery technology. Herein, a lithium‐ion cable battery is invented, which is insensitive to deformation due to its use of carbon nanotube (CNT) woven macrofilms as the charge collectors. An ultrahigh‐tap density of 10 mg cm^?2 of the electrodes can be obtained, which leads to an extremely high‐energy density of 215 mWh cm^?3. The value is approximately seven times than that of the highest performance reported previously. In addition, the battery displays very stable rate performance and lower internal resistance than conventional lithium‐ion batteries using metal charge collectors. Moreover, it demonstrates excellent convenience for connecting electronics as a new strategy is applied, in which both electrodes can be integrated into one end by a CNT macrorope. Such an ultrahigh‐energy density lithium‐ion cable battery provides a feasible way to power wearable electronics with commercial viability.     

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.     

Stretchable and Soft Electronics using Liquid Metals

The use of liquid metals based on gallium for soft and stretchable electronics is discussed. This emerging class of electronics is motivated, in part, by the new opportunities that arise from devices that have mechanical properties similar to those encountered in the human experience, such as skin, tissue, textiles, and clothing. These types of electronics (e.g., wearable or implantable electronics, sensors for soft robotics, e‐skin) must operate during deformation. Liquid metals are compelling materials for these applications because, in principle, they are infinitely deformable while retaining metallic conductivity. Liquid metals have been used for stretchable wires and interconnects, reconfigurable antennas, soft sensors, self‐healing circuits, and conformal electrodes. In contrast to Hg, liquid metals based on gallium have low toxicity and essentially no vapor pressure and are therefore considered safe to handle. Whereas most liquids bead up to minimize surface energy, the presence of a surface oxide on these metals makes it possible to pattern them into useful shapes using a variety of techniques, including fluidic injection and 3D printing. In addition to forming excellent conductors, these metals can be used actively to form memory devices, sensors, and diodes that are completely built from soft materials. The properties of these materials, their applications within soft and stretchable electronics, and future opportunities and challenges are considered.     

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.     

Biofriendly,Stretchable, and Reusable Hydrogel Electronics as Wearable Force Sensors

The ever‐growing overlap between stretchable electronic devices and wearable healthcare applications is igniting the discovery of novel biocompatible and skin‐like materials for human‐friendly stretchable electronics fabrication. Amongst all potential candidates, hydrogels with excellent biocompatibility and mechanical features close to human tissues are constituting a promising troop for realizing healthcare‐oriented electronic functionalities. In this work, based on biocompatible and stretchable hydrogels, a simple paradigm to prototype stretchable electronics with an embedded three‐dimensional (3D) helical conductive layout is proposed. Thanks to the 3D helical structure, the hydrogel electronics present satisfactory mechanical and electrical robustness under stretch. In addition, reusability of stretchable electronics is realized with the proposed scenario benefiting from the swelling property of hydrogel. Although losing water would induce structure shrinkage of the hydrogel network and further undermine the function of hydrogel in various applications, the worn‐out hydrogel electronics can be reused by simply casting it in water. Through such a rehydration procedure, the dehydrated hydrogel can absorb water from the surrounding and then the hydrogel electronics can achieve resilience in mechanical stretchability and electronic functionality. Also, the ability to reflect pressure and strain changes has revealed the hydrogel electronics to be promising for advanced wearable sensing applications.     

Stretchable Thin‐Film Electrodes for Flexible Electronics with High Deformability and Stretchability

Flexible and stretchable electronics represent today's cutting‐edge electronic technologies. As the most‐fundamental component of electronics, the thin‐film electrode remains the research frontier due to its key role in the successful development of flexible and stretchable electronic devices. Stretchability, however, is generally more challenging to achieve than flexibility. Stretchable electronic devices demand, above all else, that the thin‐film electrodes have the capacity to absorb a large level of strain (>>1%) without obvious changes in their electrical performance. This article reviews the progress in strategies for obtaining highly stretchable thin‐film electrodes. Applications of stretchable thin‐film electrodes fabricated via these strategies are described. Some perspectives and challenges in this field are also put forward.