Skin‐Like Stretchable Fuel Cell Based on Gold‐Nanowire‐Impregnated Porous Polymer Scaffolds

Skin‐like energy devices can be conformally attached to the human body, which are highly desirable to power soft wearable electronics in the future. Here, a skin‐like stretchable fuel cell based on ultrathin gold nanowires (AuNWs) and polymerized high internal phase emulsions (polyHIPEs) scaffolds is demonstrated. The polyHIPEs can offer a high porosity of 80% yet with an overall thickness comparable to human skin. Upon impregnation with electronic inks containing ultrathin (2 nm in diameter) and ultrahigh aspect‐ratio (>10 000) gold nanowires, skin‐like strain‐insensitive stretchable electrodes are successfully fabricated. With such designed strain‐insensitive electrodes, a stretchable fuel cell is fabricated by using AuNWs@polyHIPEs, platinum (Pt)‐modified AuNWs@polyHIPEs, and ethanol as the anode, cathode, and fuel, respectively. The resulting epidermal fuel cell can be patterned and transferred onto skin as “tattoos” yet can offer a high power density of 280 µW cm^?2 and a high durability (>90% performance retention under stretching, compression, and twisting). The results presented here demonstrate that this skin‐thin, porous, yet stretchable electrode is essentially multifunctional, simultaneously serving as a current collector, an electrocatalyst, and a fuel host, indicating potential applications to power future soft wearable 2.0 electronics for remote healthcare and soft robotics.     

Photosynthetic Bioelectronic Sensors for Touch Perception,UV‐Detection,and Nanopower Generation: Toward Self‐Powered E‐Skins

Energy self‐sufficiency is an inspirational design feature of biological systems that fulfills sensory functions. Plants such as the “touch‐me‐not” and “Venus flytrap” not only sustain life by photosynthesis, but also execute specialized sensory responses to touch. Photosynthesis enables these organisms to sustainably harvest and expend energy, powering their sensory abilities. Photosynthesis therefore provides a promising model for self‐powered sensory devices like electronic skins (e‐skins). While the natural sensory abilities of human skin have been emulated in man‐made materials for advanced prosthetics and soft‐robotics, no previous e‐skin has incorporated phototransduction and photosensory functions that could extend the sensory abilities of human skin. A proof‐of‐concept bioelectronic device integrated with natural photosynthetic pigment‐proteins is presented that shows the ability to sense not only touch stimuli (down to 3000 Pa), but also low‐intensity ultraviolet radiation (down to 0.01 mW cm^‐2) and generate an electrical power of ≈260 nW cm^‐2. The scalability of this device is demonstrated through the fabrication of flexible, multipixel, bioelectronic sensors capable of touch registration and tracking. The polysensory abilities, energy self‐sufficiency, and additional nanopower generation exhibited by this bioelectronic system make it particularly promising for applications like smart e‐skins and wearable sensors, where the photogenerated power can enable remote data transmission.     

EGaIn‐Assisted Room‐Temperature Sintering of Silver Nanoparticles for Stretchable,Inkjet‐Printed,Thin‐Film Electronics

Coating inkjet‐printed traces of silver nanoparticle (AgNP) ink with a thin layer of eutectic gallium indium (EGaIn) increases the electrical conductivity by six‐orders of magnitude and significantly improves tolerance to tensile strain. This enhancement is achieved through a room‐temperature “sintering” process in which the liquid‐phase EGaIn alloy binds the AgNP particles (≈100 nm diameter) to form a continuous conductive trace. Ultrathin and hydrographically transferrable electronics are produced by printing traces with a composition of AgNP‐Ga‐In on a 5 µm‐thick temporary tattoo paper. The printed circuit is flexible enough to remain functional when deformed and can support strains above 80% with modest electromechanical coupling (gauge factor ≈1). These mechanically robust thin‐film circuits are well suited for transfer to highly curved and nondevelopable 3D surfaces as well as skin and other soft deformable substrates. In contrast to other stretchable tattoo‐like electronics, the low‐cost processing steps introduced here eliminate the need for cleanroom fabrication and instead requires only a commercial desktop printer. Most significantly, it enables functionalities like “electronic tattoos” and 3D hydrographic transfer that have not been previously reported with EGaIn or EGaIn‐based biphasic electronics.     

Tattoo‐Paper Transfer as a Versatile Platform for All‐Printed Organic Edible Electronics

The use of natural or bioinspired materials to develop edible electronic devices is a potentially disruptive technology that can boost point‐of‐care testing. The technology exploits devices that can be safely ingested, along with pills or even food, and operated from within the gastrointestinal tract. Ingestible electronics can potentially target a significant number of biomedical applications, both as therapeutic and diagnostic tool, and this technology may also impact the food industry, by providing ingestible or food‐compatible electronic tags that can “smart” track goods and monitor their quality along the distribution chain. Temporary tattoo‐paper is hereby proposed as a simple and versatile platform for the integration of electronics onto food and pharmaceutical capsules. In particular, the fabrication of all‐printed organic field‐effect transistors on untreated commercial tattoo‐paper, and their subsequent transfer and operation on edible substrates with a complex nonplanar geometry is demonstrated.     

A Hierarchical Nanoparticle‐in‐Micropore Architecture for Enhanced Mechanosensitivity and Stretchability in Mechanochromic Electronic Skins

Biological tissues are multiresponsive and functional, and similar properties might be possible in synthetic systems by merging responsive polymers with hierarchical soft architectures. For example, mechanochromic polymers have applications in force‐responsive colorimetric sensors and soft robotics, but their integration into sensitive, multifunctional devices remains challenging. Herein, a hierarchical nanoparticle‐in‐micropore (NP‐MP) architecture in porous mechanochromic polymers, which enhances the mechanosensitivity and stretchability of mechanochromic electronic skins (e‐skins), is reported. The hierarchical NP‐MP structure results in stress‐concentration‐induced mechanochemical activation of mechanophores, significantly improving the mechanochromic sensitivity to both tensile strain and normal force (critical tensile strain: 50% and normal force: 1 N). Furthermore, the porous mechanochromic composites exhibit a reversible mechanochromism under a strain of 250%. This architecture enables a dual‐mode mechanochromic e‐skin for detecting static/dynamic forces via mechanochromism and triboelectricity. The hierarchical NP‐MP architecture provides a general platform to develop mechanochromic composites with high sensitivity and stretchability.     

An Artificial Flexible Visual Memory System Based on an UV‐Motivated Memristor

For the mimicry of human visual memory, a prominent challenge is how to detect and store the image information by electronic devices, which demands a multifunctional integration to sense light like eyes and to memorize image information like the brain by transforming optical signals to electrical signals that can be recognized by electronic devices. Although current image sensors can perceive simple images in real time, the image information fades away when the external image stimuli are removed. The deficiency between the state‐of‐the‐art image sensors and visual memory system inspires the logical integration of image sensors and memory devices to realize the sensing and memory process toward light information for the bionic design of human visual memory. Hence, a facile architecture is designed to construct artificial flexible visual memory system by employing an UV‐motivated memristor. The visual memory arrays can realize the detection and memory process of UV light distribution with a patterned image for a long‐term retention and the stored image information can be reset by a negative voltage sweep and reprogrammed to the same or an other image distribution, which proves the effective reusability. These results provide new opportunities for the mimicry of human visual memory and enable the flexible visual memory device to be applied in future wearable electronics, electronic eyes, multifunctional robotics, and auxiliary equipment for visual handicapped.     

Engineering the Charge Transport of Ag Nanocrystals for Highly Accurate,Wearable Temperature Sensors through All‐Solution Processes

All‐nanocrystal (NC)‐based and all‐solution‐processed wearable resistance temperature detectors (RTDs) are introduced. The charge transport mechanisms of Ag NC thin films are engineered through various ligand treatments to design high performance RTDs. Highly conductive Ag NC thin films exhibiting metallic transport behavior with high positive temperature coefficients of resistance (TCRs) are achieved through tetrabutylammonium bromide treatment. Ag NC thin films showing hopping transport with high negative TCRs are created through organic ligand treatment. All‐solution‐based, one‐step photolithography techniques that integrate two distinct opposite‐sign TCR Ag NC thin films into an ultrathin single device are developed to decouple the mechanical effects such as human motion. The unconventional materials design and strategy enables highly accurate, sensitive, wearable and motion‐free RTDs, demonstrated by experiments on moving or curved objects such as human skin, and simulation results based on charge transport analysis. This strategy provides a low cost and simple method to design wearable multifunctional sensors with high sensitivity which could be utilized in various fields such as biointegrated sensors or electronic skin.     

全印制柔性应变传感器的原理与智能包装应用

目的随着可穿戴电子技术的快速发展,因具有较高的传感系数,柔性应变传感器在电子皮肤和机器人领域得到了广泛关注,但如何降低其制造成本成为一种挑战。近年来,印刷电子技术的快速发展推动了柔性应变传感器的发展,并逐渐在一些新的领域得到应用,尤其是智能包装领域。方法结合课题组在全印制应变传感器方面的研究进展,对柔性传感器的原理、印刷制造方法和主要应用进行综述。结论大量的研究表明,印刷柔性应变传感器已经开始应用于智能包装中,利用印刷电子技术制造智能包装也有利于降低其制造成本,推动其走向实际应用。     

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.     

Soft Elastomers with Ionic Liquid‐Filled Cavities as Strain Isolating Substrates for Wearable Electronics

Managing the mechanical mismatch between hard semiconductor components and soft biological tissues represents a key challenge in the development of advanced forms of wearable electronic devices. An ultralow modulus material or a liquid that surrounds the electronics and resides in a thin elastomeric shell provides a strain‐isolation effect that enhances not only the wearability but also the range of stretchability in suitably designed devices. The results presented here build on these concepts by (1) replacing traditional liquids explored in the past, which have some nonnegligible vapor pressure and finite permeability through the encapsulating elastomers, with ionic liquids to eliminate any possibility for leakage or evaporation, and (2) positioning the liquid between the electronics and the skin, within an enclosed, elastomeric microfluidic space, but not in direct contact with the active elements of the system, to avoid any negative consequences on electronic performance. Combined experimental and theoretical results establish the strain‐isolating effects of this system, and the considerations that dictate mechanical collapse of the fluid‐filled cavity. Examples in skin‐mounted wearable include wireless sensors for measuring temperature and wired systems for recording mechano‐acoustic responses.     

Printable Fabrication of a Fully Integrated and Self‐Powered Sensor System on Plastic Substrates

Wearable and portable devices with desirable flexibility, operational safety, and long cruising time, are in urgent demand for applications in wireless communications, multifunctional entertainments, personal healthcare monitoring, etc. Herein, a monolithically integrated self‐powered smart sensor system with printed interconnects, printed gas sensor for ethanol and acetone detection, and printable supercapacitors and embedded solar cells as energy sources, is successfully demonstrated in a wearable wristband fashion by utilizing inkjet printing as a proof‐of‐concept. In such a “wearable wristband”, the harvested solar energy can either directly drive the sensor and power up a light‐emitting diode as a warning signal, or can be stored in the supercapacitors in a standby mode, and the energy released from supercapacitors can compensate the intermittency of light illumination. To the best of our knowledge, the demonstration of such a self‐powered sensor system integrated onto a single piece of flexible substrate in a printable and additive manner has not previously been reported. Particularly, the printable supercapacitors deliver an areal capacitance of 12.9 mF cm^?2 and the printed SnO₂ gas sensor shows remarkable detection sensitivity under room temperature. The printable strategies for device fabrication and system integration developed here show great potency for scalable and facile fabrication of a variety of wearable devices.     

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.     

Extraordinarily Stretchable All‐Carbon Collaborative Nanoarchitectures for Epidermal Sensors

Multifunctional microelectronic components featuring large stretchability, high sensitivity, high signal‐to‐noise ratio (SNR), and broad sensing range have attracted a huge surge of interest with the fast developing epidermal electronic systems. Here, the epidermal sensors based on all‐carbon collaborative percolation network are demonstrated, which consist 3D graphene foam and carbon nanotubes (CNTs) obtained by two‐step chemical vapor deposition processes. The nanoscaled CNT networks largely enhance the stretchability and SNR of the 3D microarchitectural graphene foams, endowing the strain sensor with a gauge factor as high as 35, a wide reliable sensing range up to 85%, and excellent cyclic stability (>5000 cycles). The flexible and reversible strain sensor can be easily mounted on human skin as a wearable electronic device for real‐time and high accuracy detecting of electrophysiological stimuli and even for acoustic vibration recognition. The rationally designed all‐carbon nanoarchitectures are scalable, low cost, and promising in practical applications requiring extraordinary stretchability and ultrahigh SNRs.     

Mechanically Flexible Conductors for Stretchable and Wearable E‐Skin and E‐Textile Devices

Considerable progress in materials development and device integration for mechanically bendable and stretchable optoelectronics will broaden the application of “Internet‐of‐Things” concepts to a myriad of new applications. When addressing the needs associated with the human body, such as the detection of mechanical functions, monitoring of health parameters, and integration with human tissues, optoelectronic devices, interconnects/circuits enabling their functions, and the core passive components from which the whole system is built must sustain different degrees of mechanical stresses. Herein, the basic characteristics and performance of several of these devices are reported, particularly focusing on the conducting element constituting them. Among these devices, strain sensors of different types, energy storage elements, and power/energy storage and generators are included. Specifically, the advances during the past 3 years are reported, wherein mechanically flexible conducting elements are fabricated from (0D, 1D, and 2D) conducting nanomaterials from metals (e.g., Au nanoparticles, Ag flakes, Cu nanowires), carbon nanotubes/nanofibers, 2D conductors (e.g., graphene, MoS₂), metal oxides (e.g., Zn nanorods), and conducting polymers (e.g., poly(3,4‐ethylenedioxythiophene):poly(4‐styrene sulfonate), polyaniline) in combination with passive fibrotic and elastomeric materials enabling, after integration, the so‐called electronic skins and electronic textiles.     

A Freestanding Stretchable and Multifunctional Transistor with Intrinsic Self‐Healing Properties of all Device Components

A flexible and stretchable field‐effect transistor (FET) is an essential element in a number of modern electronics. To realize the potential of this device in harsh real‐world conditions and to extend its application spectrum, new functionalities are needed to be introduced into the device. Here, solution‐processable elements based on carbon nanotubes that empower flexible and stretchable FET with high hole‐mobility (µ_h ≈ 10 cm² V^?1 s^?1) and relatively low operating voltages (<8 V) and that retain self‐healing properties of all FET components are reported. The device has repeatable intrinsic and autonomic self‐healing ability, namely without use of any external trigger, enabling the restoration of its electrical and mechanical properties, both after microscale damage or complete cut of the device—for example by a scissor. The device can be repeatedly stretched for >200 cycles of up to 50% strain without a significant loss in its electrical properties. The device is applicable in the form of a ≈3 µm thick freestanding skin tattoo and has multifunctional sensing properties, such as detection of temperature and humidity. With this unprecedented biomimetic transistor, highly sustainable and reliable soft electronic applications can be introduced.     

3D Printed Stretchable Tactile Sensors

The development of methods for the 3D printing of multifunctional devices could impact areas ranging from wearable electronics and energy harvesting devices to smart prosthetics and human–machine interfaces. Recently, the development of stretchable electronic devices has accelerated, concomitant with advances in functional materials and fabrication processes. In particular, novel strategies have been developed to enable the intimate biointegration of wearable electronic devices with human skin in ways that bypass the mechanical and thermal restrictions of traditional microfabrication technologies. Here, a multimaterial, multiscale, and multifunctional 3D printing approach is employed to fabricate 3D tactile sensors under ambient conditions conformally onto freeform surfaces. The customized sensor is demonstrated with the capabilities of detecting and differentiating human movements, including pulse monitoring and finger motions. The custom 3D printing of functional materials and devices opens new routes for the biointegration of various sensors in wearable electronics systems, and toward advanced bionic skin applications.     

Thread‐like Supercapacitors Based on One‐Step Spun Nanocomposite Yarns

Thread‐like electronic devices have attracted great interest because of their potential applications in wearable electronics. To produce high‐performance, thread‐like supercapacitors, a mixture of stable dispersions of single‐walled carbon nanotubes and conducting polyaniline nanowires are prepared. Then, the mixture is spun into flexible yarns with a polyvinyl alcohol outer sheath by a one‐step spinning process. The composite yarns show excellent mechanical properties and high electrical conductivities after sufficient washing to remove surfactants. After applying a further coating layer of gel electrolyte, two flexible yarns are twisted together to form a thread‐like supercapacitor. The supercapacitor based on these two yarns (SWCNTs and PAniNWs) possesses a much higher specific capacitance than that based only on pure SWCNTs yarns, making it an ideal energy‐storage device for wearable electronics.     

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.     

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.     

Stimulus Responsive 3D Assembly for Spatially Resolved Bifunctional Sensors

3D electronic/optoelectronic devices have shown great potentials for various applications due to their unique properties inherited not only from functional materials, but also from 3D architectures. Although a variety of fabrication methods including mechanically guided assembly have been reported, the resulting 3D devices show no stimuli‐responsive functions or are not free standing, thereby limiting their applications. Herein, the stimulus responsive assembly of complex 3D structures driven by temperature‐responsive hydrogels is demonstrated for applications in 3D multifunctional sensors. The assembly driving force, compressive buckling, arises from the volume shrinkage of the responsive hydrogel substrates when they are heated above the lower critical solution temperature. Driven by the compressive buckling force, the 2D‐formed membrane materials, which are pre‐defined and selectively bonded to the substrates, are then assembled to 3D structures. They include “tent,” “tower,” “two‐floor pavilion,” “dome,” “basket,” and “nested‐cages” with delicate geometries. Moreover, the demonstrated 3D bifunctional sensors based on laser induced graphene show capability of spatially resolved tactile sensing and temperature sensing. These multifunctional 3D sensors would open new applications in soft robotics, bioelectronics, micro‐electromechanical systems, and others.