Light‐Powered Healing of a Wearable Electrical Conductor

Mechanical failure along a conductive pathway can cause unexpected shutdown of an electronic devices, ultimately limiting the device lifetime. To address this problem, various systems to realize healable electrical conductors have been proposed; however, rapid, noninvasive, and on‐demand healing, factors that are all synergistically required, especially for wearable device applications, still remains challenging. Here, a light‐powered healable electrical conductor (conceptualized as photofluidic diffusional system) is proposed for simple‐, fast‐, and easy‐to‐implement wearable devices (e.g., the electronic skin, sensitive to mechanical motion). Contrary to other implementations such as capsules, heat, water, and mechanical forces, green light even with low intensity has potential to provide fast (less than 3 min) and repetitive recovery of a damaged electrical conductor without any direct invasion. Also, the multiple, irregular cracks resulting from vigorous motions of wearable devices can be simultaneously recovered regardless of the light incident angles and crack propagation directions, thus, making light‐powered healing more accessible to wearable devices beyond existing system options. To develop and demonstrate the key concepts of this system, combined studies on materials, integrations, and light‐powering strategy for recovering a damaged wearable electrical conductor are systematically carried out in the present work.     

An Amphiphobic Hydraulic Triboelectric Nanogenerator for a Self‐Cleaning and Self‐Charging Power System

Raindrop falling, which is one kind of water motions, contains large amount of mechanical energy. However, harvesting energy from the falling raindrop to drive electronics continuously is not commonly investigated. Therefore, a self‐cleaning/charging power system (SPS) is reported, which can be exploited to convert and store energy from falling raindrop directly for providing a stable and durable output. The SPS consists of a hydraulic triboelectric nanogenerator (H‐TENG) and several embedded fiber supercapacitors. The surface of H‐TENG is amphiphobic, enabling the SPS self‐cleaning. The fiber supercapacitor which uses α‐Fe₂O₃/reduced graphene oxide composite possesses remarkable specific capacitance, excellent electrical stability, and high flexibility. These properties of the fiber supercapacitor make it suitable for a wearable power system. A power raincoat based on the SPS is demonstrated as application. After showering by water flow, which simulates falling raindrops, for 100 s, the power raincoat achieves an open‐circuit voltage of 4 V and lights a light‐emitting diode for more than 300 s. With features of low cost, easy installation, and good flexibility, the SPS harvesting energy from the falling raindrop renders as a promising sustainable power source for wearable and portable electronics.     

3D‐Printed All‐Fiber Li‐Ion Battery toward Wearable Energy Storage

Conventional bulky and rigid power systems are incapable of meeting flexibility and breathability requirements for wearable applications. Despite the tremendous efforts dedicated to developing various 1D energy storage devices with sufficient flexibility, challenges remain pertaining to fabrication scalability, cost, and efficiency. Here, a scalable, low‐cost, and high‐efficiency 3D printing technology is applied to fabricate a flexible all‐fiber lithium‐ion battery (LIB). Highly viscous polymer inks containing carbon nanotubes and either lithium iron phosphate (LFP) or lithium titanium oxide (LTO) are used to print LFP fiber cathodes and LTO fiber anodes, respectively. Both fiber electrodes demonstrate good flexibility and high electrochemical performance in half‐cell configurations. All‐fiber LIB can be successfully assembled by twisting the as‐printed LFP and LTO fibers together with gel polymer as the quasi‐solid electrolyte. The all‐fiber device exhibits a high specific capacity of ≈110 mAh g^?1 at a current density of 50 mA g^?1 and maintains a good flexibility of the fiber electrodes, which can be potentially integrated into textile fabrics for future wearable electronic applications.     

Inkjet Printed Large‐Area Flexible Few‐Layer Graphene Thermoelectrics

Graphene‐based organic nanocomposites have ascended as promising candidates for thermoelectric energy conversion. In order to adopt existing scalable printing methods for developing thermostable graphene‐based thermoelectric devices, optimization of both the material ink and the thermoelectric properties of the resulting films are required. Here, inkjet‐printed large‐area flexible graphene thin films with outstanding thermoelectric properties are reported. The thermal and electronic transport properties of the films reveal the so‐called phonon‐glass electron‐crystal character (i.e., electrical transport behavior akin to that of few‐layer graphene flakes with quenched thermal transport arising from the disordered nanoporous structure). As a result, the all‐graphene films show a room‐temperature thermoelectric power factor of 18.7 µW m^?1 K^?2, representing over a threefold improvement to previous solution‐processed all‐graphene structures. The demonstration of inkjet‐printed thermoelectric devices underscores the potential for future flexible, scalable, and low‐cost thermoelectric applications, such as harvesting energy from body heat in wearable applications.     

Healable Transparent Electronic Devices

With the advent of the digital era, healable electronic devices are being developed to alleviate the propagation of breakdown in electronics due to the mechanical damage caused by bending, accidental cutting or scratching. Meanwhile, flexible transparent electronics, exhibiting high transmittance and robust flexibility, are drawing enormous research efforts due to their potential applications in various integrated wearable electronics. However, the breakdown of flexible transparent electronics seriously limits their reliability and lifetime. Therefore, transparent healable electronics are desired to tackle these problems, yet most of the healable electronics are not transparent nowadays. The combination of high performance, healability, and transparency into electronics is often mutually exclusive. Herein, after a brief introduction of self‐healing materials, healable electronics, and flexible transparent electronics, the recent progress in the healable electronic devices without transparency is reviewed in detail. Then, healable transparent electronic devices with high transparency, robust portability, and reliable flexibility are summarized. They are drawing great attention owing to their potential application in optical devices as well as smart wearable and integrated optoelectronic devices. Following that, the critical challenges and prospects are highlighted for the development of healable transparent electronic devices.     

Self‐Healable and Stretchable Organic Thermoelectric Materials: Electrically Percolated Polymer Nanowires Embedded in Thermoplastic Elastomer Matrix

Self‐healable and stretchable energy‐harvesting materials can provide a new avenue for the realization of self‐powered wearable electronics, including electronic skins, whose main materials are required to be robust to and stable under external damage and severe mechanical stresses. However, thermoelectric (TE) materials showing both self‐healing properties and stretchability have not yet been demonstrated despite their great potential to harvest thermal energy in the human body. As most existing TE materials are either mechanically brittle or unrecoverable after being subjected to damage, a novel approach is necessary for designing such materials. Herein, self‐healable and stretchable TE materials based on all‐organic composite system wherein polymer semiconductor nanowires are p‐doped with a molecular dopant and embedded in a thermoplastic elastomer matrix are reported. The polymer nanowires are electrically percolated in the matrix, and the resulting composite materials exhibit good TE performance. The composites also exhibit both excellent self‐healing properties under mild heat and pressure conditions and good stretchability. It is believed that this work can be a cornerstone for the design of self‐healable and stretchable energy‐harvesting materials as it provides useful guidelines for imparting electrical conductivity to insulating thermoplastic elastomers, which typically possess versatile and useful mechanical properties.     

Self‐Healing and Stretchable 3D‐Printed Organic Thermoelectrics

With the advent of flexible and wearable electronics and sensors, there is an urgent need to develop energy‐harvesting solutions that are compatible with such wearables. However, many of the proposed energy‐harvesting solutions lack the necessary mechanical properties, which make them susceptible to damage by repetitive and continuous mechanical stresses, leading to serious degradation in device performance. Developing new energy materials that possess high deformability and self‐healability is essential to realize self‐powered devices. Herein, a thermoelectric ternary composite is demonstrated that possesses both self‐healing and stretchable properties produced via 3D‐printing method. The ternary composite films provide stable thermoelectric performance during viscoelastic deformation, up to 35% tensile strain. Importantly, after being completely severed by cutting, the composite films autonomously recover their thermoelectric properties with a rapid response time of around one second. Using this self‐healable and solution‐processable composite, 3D‐printed thermoelectric generators are fabricated, which retain above 85% of their initial power output, even after repetitive cutting and self‐healing. This approach represents a significant step in achieving damage‐free and truly wearable 3D‐printed organic thermoelectrics.     

A Mediator‐Free Electroenzymatic Sensing Methodology to Mitigate Ionic and Electroactive Interferents' Effects for Reliable Wearable Metabolite and Nutrient Monitoring

Wearable electroenzymatic sensors enable monitoring of clinically informative biomolecules in epidermally retrievable biofluids. Conventional wearable enzymatic sensors utilize Prussian Blue (a redox mediator) to achieve selectivity against electroactive interferents. However, the use of Prussian Blue presents fundamental challenges including: 1) the susceptibility of the sensor response to dynamic concentration variation of ionic species and 2) the poor operational stability due to the degradation of its framework. As an alternative wearable electroenzymatic sensor development methodology to bypass the aforementioned limitations, a mediator‐free sensing interface is devised, comprising of a coupled platinum nanoparticle/multiwall carbon nanotube layer and a permselective membrane. The interface is adapted to develop sensors targeting glucose, lactate, and choline (as examples of informative metabolites and nutrients), showing high degrees of sensitivity, selectivity (against a wide panel of naturally present and diverse interfering species), stability (<6.5% signal drift over 20 h operation), and reliability of sensing operation in sweat samples. By integration within a readout board, a wireless sample‐to‐answer system is realized for on‐body sweat biomarker analysis. This methodology can be adapted to target a wide panel of biomarkers in various biofluids, introducing a new sensor development direction for personal health monitoring.     

Recent Developments of Planar Micro‐Supercapacitors: Fabrication,Properties, and Applications

The increasing development of wearable, portable, implantable, and highly integrated electronic devices has led to an increasing demand for miniaturization of energy storage devices. In recent years, supercapacitors, as an energy storage device, have received enormous attention owing to their excellent properties of quick charge and discharge, high power density, and long life cycle with minimal maintenance. Micro‐supercapacitors (MSCs) as a promising candidate for miniaturized energy storage components have undergone considerable theoretical and experimental investigations. Particularly, planar MSCs with a 2D architecture design have more attractive application prospects due to their flexible design and excellent electrochemical performance. However, the major drawbacks of MSCs are their intrinsically low energy density. For this reason, researchers have conducted much investigation to improve their energy density in order to promote their practical application. Herein, the recent development and progress of planar MSCs from the scope of the substrates, electrode materials, fabrication methods, electrochemical properties, and applications are discussed. Finally, the currently existing challenges and developments associated with planar MSCs are also discussed. All in all, planar MSCs have great application potential in various fields of electrochemical energy storage, self‐powered wireless sensors, and stimuli‐responsive and photoresponsive, alternating current line filtering.     

In‐Plane Micro‐Supercapacitors for an Integrated Device on One Piece of Paper

Portable and wearable sensors have attracted considerable attention in the healthcare field because they can be worn or implanted into a human body to monitor environmental information. However, sensors cannot work independently and require power. Flexible in‐plane micro‐supercapacitor (MSC) is a suitable power device that can be integrated with sensors on a single chip. Meanwhile, paper is an ideal flexible substrate because it is cheap and disposable and has a porous and rough surface that enhances interface adhesion with electronic devices. In this study, a new strategy to integrate MSCs, which have excellent electrochemical and mechanical performances, with sensors on a single piece of paper is proposed. The integration is achieved by printing Ni circuit on paper without using a precoating underlay. Ink diffusion is also addressed to some degree. Meanwhile, a UV sensor is integrated on a single paper, and the as‐integrated device shows good sensing and self‐powering capabilities. MSCs can also be integrated with a gas sensor on one‐piece paper and can be charged by connecting it to a solar cell. Thus, it is potentially feasible that a flexible paper can be used for integrating MSCs with solar cell and various sensors to generate, store, and use energy.     

Fingerprint‐Inspired Conducting Hierarchical Wrinkles for Energy‐Harvesting E‐Skin

In the field of bionics, sophisticated and multifunctional electronic skins with a mechanosensing function that are inspired by nature are developed. Here, an energy‐harvesting electronic skin (energy‐E‐skin), i.e., a pressure sensor with energy‐harvesting functions is demonstrated, based on fingerprint‐inspired conducting hierarchical wrinkles. The conducting hierarchical wrinkles, fabricated via 2D stretching and subsequent Ar plasma treatment, are composed of polydimethylsiloxane (PDMS) wrinkles as the primary microstructure and embedded Ag nanowires (AgNWs) as the secondary nanostructure. The structure and resistance of the conducting hierarchical wrinkles are deterministically controlled by varying the stretching direction, Ar plasma power, and treatment time. This hierarchical‐wrinkle‐based conductor successfully harvests mechanical energy via contact electrification and electrostatic induction and also realizes self‐powered pressure sensing. The energy‐E‐skin delivers an average output power of 3.5 mW with an open‐circuit voltage of 300 V and a short‐circuit current of 35 µA; this power is sufficient to drive commercial light‐emitting diodes and portable electronic devices. The hierarchical‐wrinkle‐based conductor is also utilized as a self‐powered tactile pressure sensor with a sensitivity of 1.187 mV Pa^‐1 in both contact‐separation mode and the single‐electrode mode. The proposed energy‐E‐skin has great potential for use as a next‐generation multifunctional artificial skin, self‐powered human–machine interface, wearable thin‐film power source, and so on.     

Waterproof,Breathable, and Antibacterial Self‐Powered e‐Textiles Based on Omniphobic Triboelectric Nanogenerators

Multifunctional electronic textiles (e‐textiles) incorporating miniaturized electronic devices will pave the way toward a new generation of wearable devices and human–machine interfaces. Unfortunately, the development of e‐textiles is subject to critical challenges, such as battery dependence, breathability, satisfactory washability, and compatibility with mass production techniques. This work describes a simple and cost‐effective method to transform conventional garments and textiles into waterproof, breathable, and antibacterial e‐textiles for self‐powered human–machine interfacing. Combining embroidery with the spray‐based deposition of fluoroalkylated organosilanes and highly networked nanoflakes, omniphobic triboelectric nanogenerators (R^F‐TENGs) can be incorporated into any fiber‐based textile to power wearable devices using energy harvested from human motion. R^F‐TENGs are thin, flexible, breathable (air permeability 90.5 mm s^?1), inexpensive to fabricate (<0.04$ cm^?2), and capable of producing a high power density (600 µW cm^?2). E‐textiles based on R^F‐TENGs repel water, stains, and bacterial growth, and show excellent stability under mechanical deformations and remarkable washing durability under standard machine‐washing tests. Moreover, e‐textiles based on R^F‐TENGs are compatible with large‐scale production processes and exhibit high sensitivity to touch, enabling the cost‐effective manufacturing of wearable human–machine interfaces.     

Wood‐Derived Materials for Advanced Electrochemical Energy Storage Devices

Over the past decade, wood‐derived materials have attracted enormous interest for both fundamental research and practical applications in various functional devices. In addition to being renewable, environmentally benign, naturally abundant, and biodegradable, wood‐derived materials have several unique advantages, including hierarchically porous structures, excellent mechanical flexibility and integrity, and tunable multifunctionality, making them ideally suited for efficient energy storage and conversion. In this article, the latest advances in the development of wood‐derived materials are discussed for electrochemical energy storage systems and devices (e.g., supercapacitors and rechargeable batteries), highlighting their micro/nanostructures, strategies for tailoring the structures and morphologies, as well as their impact on electrochemical performance (energy and power density and long‐term durability). Furthermore, the scientific and technical challenges, together with new directions of future research in this exciting field, are also outlined for electrochemical energy storage applications.     

Stretchable Energy‐Harvesting Tactile Interactive Interface with Liquid‐Metal‐Nanoparticle‐Based Electrodes

Energy‐harvesting electronic skin (E‐skin) is highly promising for sustainable and self‐powered interactive systems, wearable human health monitors, and intelligent robotics. Flexible/stretchable electrodes and robust energy‐harvesting components are critical in constructing soft, wearable, and energy‐autonomous E‐skin systems. A stretchable energy‐harvesting tactile interactive interface is demonstrated using liquid metal nanoparticles (LM‐NPs)‐based electrodes. This stretchable energy‐harvesting tactile interface relies on triboelectric nanogenerator composed of a galinstan LM‐NP‐based stretchable electrode and patterned elastic polymer friction and encapsulation layer. It provides stable and high open‐circuit voltage (268 V), short‐circuit current (12.06 µA), and transferred charges (103.59 nC), which are sufficient to drive commercial portable electronics. As a self‐powered tactile sensor, it presents satisfactory and repeatable sensitivity of 2.52 V·kPa^?1 and is capable of working as a touch interactive keyboard. The demonstrated stretchable and robust energy‐harvesting E‐skin using LM‐NP‐based electrodes is of great significance in sustainable human–machine interactive system, intelligent robotic skin, security tactile switches, etc.     

Textile‐Based Triboelectric Nanogenerators for Self‐Powered Wearable Electronics

Wearable smart electronic devices based on wireless systems use batteries as a power source. However, recent miniaturization and various functions have increased energy consumption, resulting in problems such as reduction of use time and frequent charging. These factors hinder the development of wearable electronic devices. In order to solve this energy problem, research studies on triboelectric nanogenerators (TENGs) are conducted based on the coupling of contact‐electrification and electrostatic induction effects for harvesting the vast amounts of biomechanical energy generated from wearer movement. The development of TENGs that use a variety of structures and materials based on the textile platform is reviewed, including the basic components of fibers, yarns, and fabrics made using various weaving and knitting techniques. These textile‐based TENGs are lightweight, flexible, highly stretchable, and wearable, so that they can effectively harvest biomechanical energy without interference with human motion, and can be used as activity sensors to monitor human motion. Also, the main application of wearable self‐powered systems is demonstrated and the directions of future development of textile‐based TENG for harvesting biomechanical energy presented.     

Protein Gel Phase Transition: Toward Superiorly Transparent and Hysteresis‐Free Wearable Electronics

The next generation of wearable electronics for health monitoring, Internet‐of‐Things system, “interface‐on‐invisible,” and green energy harvesting require electrically conductive material that is superiorly transparent, negligibly hysteretic, industrially feasible, and highly stretchable. The practical potential of ionic hydrogel is challenged with obvious hysteresis and a limited sensing range due to relative delamination and viscoelastic performance. Herein, a novel liquid conductor, termed as egg white liquid, is developed from self‐liquidation of egg white hydrogel, and the liquid not only inherits the designed architecture from a hydrogel predecessor but also achieves comparable conductivity (20.4 S m^?1) to the ionic hydrogel and ultrahigh transparency (up to 99.8%) . Moreover, the 3D‐printed liquid–elastomer hybrid exhibits excellent conformability, remarkable sensitivity with negligible hysteresis (0.77%), and the capability of monitoring human motions and dynamic moduli is further demonstrated. The liquid nature inspires a gesture‐controlled touchless user interface for front‐end electronic systems. Furthermore, mechanical energy harvesting and pressure sensing are evidenced by exploiting this liquid conductor into a triboelectric nanogenerator. Notably, the as‐prepared liquid via subsequent phase transition possessing superior transparency, ultralow hysteresis, economic benefit, and unique liquid phase may potentially fuel the development of a new class of wearable electronics, human–machine interface, and clean energy.     

3D Printed High‐Loading Lithium‐Sulfur Battery Toward Wearable Energy Storage

Wearable electronic devices are the new darling of consumer electronics, and energy storage devices are an important part of them. Here, a wearable lithium‐sulfur (Li‐S) bracelet battery using three‐dimensional (3D) printing technology (additive manufacturing) is designed and manufactured for the first time. The bracelet battery can be easily worn to power the wearable device. The “additive” manufacturing characteristic of 3D printing provides excellent controllability of the electrode thickness with much simplified process in a cost‐effective manner. Due to the conductive 3D skeleton providing interpenetrating transmission paths and channels for electrons and ions, the 3D Li‐S battery can provide 505.4 mAh g^?1 specific capacity after 500 cycles with an active material loading as high as 10.2 mg cm^?1. The practicality is illustrated by wearing the bracelet battery on the wrist and illuminating the red light‐emitting diode. Therefore, the bracelet battery manufactured by 3D printing technology can address the needs of the wearable power supply.     

Single‐Thread‐Based Wearable and Highly Stretchable Triboelectric Nanogenerators and Their Applications in Cloth‐Based Self‐Powered Human‐Interactive and Biomedical Sensing

The development of wearable and large‐area fabric energy harvester and sensor has received great attention due to their promising applications in next‐generation autonomous and wearable healthcare technologies. Here, a new type of “single” thread‐based triboelectric nanogenerator (TENG) and its uses in elastically textile‐based energy harvesting and sensing have been demonstrated. The energy‐harvesting thread composed by one silicone‐rubber‐coated stainless‐steel thread can extract energy during contact with skin. With sewing the energy‐harvesting thread into a serpentine shape on an elastic textile, a highly stretchable and scalable TENG textile is realized to scavenge various kinds of human‐motion energy. The collected energy is capable to sustainably power a commercial smart watch. Moreover, the simplified single triboelectric thread can be applied in a wide range of thread‐based self‐powered and active sensing uses, including gesture sensing, human‐interactive interfaces, and human physiological signal monitoring. After integration with microcontrollers, more complicated systems, such as wireless wearable keyboards and smart beds, are demonstrated. These results show that the newly designed single‐thread‐based TENG, with the advantage of interactive, responsive, sewable, and conformal features, can meet application needs of a vast variety of fields, ranging from wearable and stretchable energy harvesters to smart cloth‐based articles.     

A High‐Reliability Kevlar Fiber‐ZnO Nanowires Hybrid Nanogenerator and its Application on Self‐Powered UV Detection

A microfiber‐nanowire hybrid structure is the fundamental component for a wearable piezoelectric nanogenerator (PENG) for harvesting body motion energy. Here, a novel approach combining surface coating and plasma etching techniques is reported to enhance the mechanical reliability of Kevlar microfiber‐ZnO nanowires (NWs) hybrid structure that is used for PENG. After treatment, the hybrid structure has dramatically improved high flexibility, robustness, and durability. On the basis of the coupled piezoelectric and semiconducting properties of ZnO, the processed Kevlar fibers covered with ZnO NWs are utilized to fabricate a 2D nanogenerator (2DNG). The open‐circuit voltage and short‐circuit current of the 2DNG are 1.8 mV and 4.8 pA, respectively. Furthermore, the 2DNG is successfully employed to quantitatively detect UV intensity from 0.2 to 1 mW cm^?2 as a self‐powered system.     

Liquid Metal Based Island‐Bridge Architectures for All Printed Stretchable Electrochemical Devices

The adoption of epidermal electronics into everyday life requires new design and fabrication paradigms, transitioning away from traditional rigid, bulky electronics towards soft devices that adapt with high intimacy to the human body. Here, a new strategy is reported for fabricating achieving highly stretchable “island‐bridge” (IB) electrochemical devices based on thick‐film printing process involving merging the deterministic IB architecture with stress‐enduring composite silver (Ag) inks based on eutectic gallium‐indium particles (EGaInPs) as dynamic electrical anchors within the inside the percolated network. The fabrication of free‐standing soft Ag‐EGaInPs‐based serpentine “bridges” enables the printed microstructures to maintain mechanical and electrical properties under an extreme (≈800%) strain. Coupling these highly stretchable “bridges” with rigid multifunctional “island” electrodes allows the realization of electrochemical devices that can sustain high mechanical deformation while displaying an extremely attractive and stable electrochemical performance. The advantages and practical utility of the new printed Ag‐liquid metal‐based island‐bridge designs are discussed and illustrated using a wearable biofuel cell. Such new scalable and tunable fabrication strategy will allow to incorporate a wide range of materials into a single device towards a wide range of applications in wearable electronics.