High‐Energy Asymmetric Supercapacitor Yarns for Self‐Charging Power Textiles

Rapid growth of electronic textile increases the demand for textile‐based power sources, which should have comparable lightweight, flexibility, and comfort. In this work, a self‐charging power textile interwoven by all‐yarn‐based energy‐harvesting triboelectric nanogenerators (TENG) and energy‐storing yarn‐type asymmetric supercapacitors (Y‐ASC) is reported. Common polyester yarns with conformal Ni/Cu coating are utilized as 1D current collectors in Y‐ASCs and electrodes in TENGs. The solid‐state Y‐ASC achieves high areal energy density (≈78.1 µWh cm^?2), high power density (14 mW cm^?2), stable cycling performance (82.7% for 5000 cycles), and excellent flexibility (1000 cycles bending for 180°). The TENG yarn can be woven into common fabrics with desired stylish designs to harvest energy from human daily motions at high output (≈60 V open‐circuit voltage and ≈3 µA short‐circuit current). The integrated self‐charging power textile is demonstrated to power an electronic watch without extra recharging by other power sources, suggesting its promising applications in electronic textiles and wearable electronics.     

High‐Performance Polypyrrole/Graphene/SnCl2 Modified Polyester Textile Electrodes and Yarn Electrodes for Wearable Energy Storage

Flexible supercapacitors have potential for wearable energy storage due to their high energy/power densities and long operating lifetimes. High electrochemical performance with robust mechanical properties is highly desired for flexible supercapacitor electrodes. Usually, the mechanical properties are improved by choosing high flexible textile substrates but at the much expense of electrochemical performance due to the nonideal contact between conductive materials and textile substrates. Herein, the authors present an efficient, scalable, and general strategy for the simultaneous fabrication of high‐performance textile electrodes and yarn electrodes. It is interesting to find that the conformal reduced graphene oxide (RGO) layer is uniformly and successively painted on the surface of SnCl₂ modified polyester fibers (M‐PEF) via a repeated “dyeing and drying” strategy. The large‐area textile electrodes and ultralong yarn electrodes are fabricated by using RGO/M‐PEF as substrate with subsequent deposition of polypyrrole. This work provides new opportunities for developing high flexible textile electrodes and yarn electrodes with further increased electrochemical performance and scalable production.     

Knittable and Washable Multifunctional MXene‐Coated Cellulose Yarns

Textile‐based electronics enable the next generation of wearable devices, which have the potential to transform the architecture of consumer electronics. Highly conductive yarns that can be manufactured using industrial‐scale processing and be washed like everyday yarns are needed to fulfill the promise and rapid growth of the smart textile industry. By coating cellulose yarns with Ti₃C₂T_x MXene, highly conductive and electroactive yarns are produced, which can be knitted into textiles using an industrial knitting machine. It is shown that yarns with MXene loading of ≈77 wt% (≈2.2 mg cm^?1) have conductivity of up to 440 S cm^?1. After washing for 45 cycles at temperatures ranging from 30 to 80 °C, MXene‐coated cotton yarns exhibit a minimal increase in resistance while maintaining constant MXene loading. The MXene‐coated cotton yarn electrode offers a specific capacitance of 759.5 mF cm^?1 at 2 mV s^?1. A fully knitted textile‐based capacitive pressure sensor is also prepared, which offers high sensitivity (gauge factor of ≈6.02), wide sensing range of up to ≈20% compression, and excellent cycling stability (2000 cycles at ≈14% compression strain). This work provides new and practical insights toward the development of platform technology that can integrate MXene in cellulose‐based yarns for textile‐based devices.     

Highly Conductive Carbon Nanotube‐Graphene Hybrid Yarn

An efficient procedure for the fabrication of highly conductive carbon nanotube/graphene hybrid yarns has been developed. To start, arrays of vertically aligned multi‐walled carbon nanotubes (MWNT) are converted into indefinitely long MWNT sheets by drawing. Graphene flakes are then deposited onto the MWNT sheets by electrospinning to form a composite structure that is transformed into yarn filaments by twisting. The process is scalable for yarn fabrication on an industrial scale. Prepared materials are characterized by electron microscopy, electrical, mechanical, and electrochemical measurements. It is found that the electrical conductivity of the composite MWNT‐graphene yarns is over 900 S/cm. This value is 400% and 1250% higher than electrical conductivity of pristine MWNT yarns or graphene paper, respectively. The increase in conductivity is asssociated with the increase of the density of states near the Fermi level by a factor of 100 and a decrease in the hopping distance by an order of magnitude induced by grapene flakes. It is found also that the MWNT‐graphene yarn has a strong electrochemical response with specific capacitance in excess of 111 Fg^?1. This value is 425% higher than the capacitance of pristine MWNT yarn. Such substantial improvements of key properties of the hybrid material can be associated with the synergy of MWNT and graphene layers in the yarn structure. Prepared hybrid yarns can benefit such applications as high‐performance supercapacitors, batteries, high current capable cables, and artificial muscles.     

Self‐Powered Electronics by Integration of Flexible Solid‐State Graphene‐Based Supercapacitors with High Performance Perovskite Hybrid Solar Cells

To develop high‐capacitance flexible solid‐state supercapacitors and explore its application in self‐powered electronics is one of ongoing research topics. In this study, self‐stacked solvated graphene (SSG) films are reported that have been prepared by a facile vacuum filtration method as the free‐standing electrode for flexible solid‐state supercapacitors. The highly hydrated SSG films have low mass loading, high flexibility, and high electrical conductivity. The flexible solid‐state supercapacitors based on SSG films exhibit excellent capacitive characteristics with a high gravimetric specific capacitance of 245 F g^?1 and good cycling stability of 10 000 cycles. Furthermore, the flexible solid‐state supercapacitors are integrated with high performance perovskite hybrid solar cells (pero‐HSCs) to build self‐powered electronics. It is found that the solid‐state supercapacitors can be charged by pero‐HSCs and discharged from 0.75 V. These results demonstrate that the self‐powered electronics by integration of the flexible solid‐state supercapacitors with pero‐HSCs have great potential applications in storage of solar energy and in flexible electronics, such as portable and wearable personal devices.     

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.     

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.     

Advances on Emerging Materials for Flexible Supercapacitors: Current Trends and Beyond

The progressive size reduction of electronic components is experiencing bottlenecks in shrinking charge storage devices like batteries and supercapacitors, limiting their development into wearable and flexible zero‐pollution technologies. The inherent long cycle life, rapid charge–discharge patterns, and power density of supercapacitors rank them superior over other energy storage devices. In the modern market of zero‐pollution energy devices, currently the lightweight formula and shape adaptability are trending to meet the current requirement of wearables. Carbon nanomaterials have the potential to meet this demand, as they are the core of active electrode materials for supercapacitors and texturally tailored to demonstrate flexible and stretchable properties. With this perspective, the latest progress in novel materials from conventional carbons to recently developed and emerging nanomaterials toward lightweight stretchable active compounds for flexi‐wearable supercapacitors is presented. In addition, the limitations and challenges in realizing wearable energy storage systems and integrating the future of nanomaterials for efficient wearable technology are provided. Moreover, future perspectives on economically viable materials for wearables are also discussed, which could motivate researchers to pursue fabrication of cheap and efficient flexible nanomaterials for energy storage and pave the way for enabling a wide‐range of material‐based applications.     

Making Stretchable Hybrid Supercapacitors by Knitting Non‐Stretchable Metal Fibers

To obtain supercapacitors for wearable electronic devices, highly conductive stretchable electrode substrates with excellent tensile recovery are required. However, the simultaneous realization of the above mentioned characteristics is difficult. In this study, tough stainless‐steel fibers (SSFs) are employed as the substrates for knitting into stainless‐steel meshes (SSMs), for the fabrication of textile electrodes with typical 2D‐interconnected networks. The obtained knitted networks can transform the angular elasticity of SSFs into the stretchability of the textile electrodes. The electrodes based on the SSM substrates can be obtained via the in situ growth of NiCo₂S₄ nanosheets covered by CoS₂ nanowires, which exhibit a high specific capacity, high rate capability, and excellent cycling stability. Moreover, the first stretchable solid‐state hybrid supercapacitors based on SSM display excellent performances with respect to a high energy density (60.2 Wh kg^?1 at 800 W kg^?1), remarkable tensile recovery (≤40% elongation), and high stability (≈76.4% capacity retention at 30% strain for 1000 stretching cycles). The highly stretchable supercapacitor is sewn on the elbow of a garment to drive a light‐emitting diode, and it maintains a high performance with respect to the repetitive process of bending and straightening, thus demonstrating the high applicability of the designed SSMs to wearable electronics.     

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.     

Flexible and Wire‐Shaped Micro‐Supercapacitor Based on Ni(OH)2‐Nanowire and Ordered Mesoporous Carbon Electrodes

Portable and multifunctional electronic devices are developing in the trend of being small, flexible, roll‐up, and even wearable, which asks us to develop flexible and micro‐sized energy conversion/storage devices. Here, the high performance of a flexible, wire‐shaped, and solid‐state micro‐supercapacitor, which is prepared by twisting a Ni(OH)2‐nanowire fiber‐electrode and an ordered mesoporous carbon fiber‐electrode together with a polymer electrolyte, is demonstrated. This micro‐supercapacitor displays a high specific capacitance of 6.67 mF cm^–1 (or 35.67 mF cm^–2) and a high specific energy density of 0.01 mWh cm^–2 (or 2.16 mWh cm^–3), which are about 10–100 times higher than previous reports. Furthermore, its capacitance retention is 70% over 10 000 cycles, indicating perfect cyclic ability. Two wire‐shaped micro‐supercapacitors (0.6 mm in diameter, ≈3 cm in length) in series can successfully operate a red light‐emitting‐diode, indicating promising practical application. Furthermore, synchrotron radiation X‐ray computed microtomo­graphy technology is employed to investigate inner structure of the micro‐device, confirming its solid‐state characteristic. This micro‐supercapacitor may bring new design opportunities of device configuration for energy‐storage devices in the future wearable electronic area.     

Wearable Self-Powered Electrochemical Devices for Continuous Health Management

The wearable revolution is already present in society through numerous gadgets. However, the contest remains in fully deployable wearable (bio)chemical sensing. Its use is constrained by the energy consumption which is provided by miniaturized batteries, limiting the autonomy of the device. Hence, the combination of materials and engineering efforts to develop sustainable energy management is paramount in the next generation of wearable self-powered electrochemical devices (WeSPEDs). In this direction, this review highlights for the first time the incorporation of innovative energy harvesting technologies with top-notch wearable self-powered sensors and low-powered electrochemical sensors toward battery-free and self-sustainable devices for health and wellbeing management. First, current elements such as wearable designs, electrochemical sensors, energy harvesters and storage, and user interfaces that conform WeSPEDs are depicted. Importantly, the bottlenecks in the development of WeSPEDs from an analytical perspective, product side, and power needs are carefully addressed. Subsequently, energy harvesting opportunities to power wearable electrochemical sensors are discussed. Finally, key findings that will enable the next generation of wearable devices are proposed. Overall, this review aims to bring new strategies for an energy-balanced deployment of WeSPEDs for successful monitoring of (bio)chemical parameters of the body toward personalized, predictive, and importantly, preventive healthcare.     

Engineering MoS2 Nanosheets on Spindle‐Like α‐Fe2O3 as High‐Performance Core–Shell Pseudocapacitive Anodes for Fiber‐Shaped Aqueous Lithium‐Ion Capacitors

Fiber‐shaped aqueous lithium‐ion capacitors (FALICs) featured with high energy and power densities together with outstanding safety characteristics are emerging as promising electrochemical energy‐storage devices for future portable and wearable electronics. However, the lack of high‐capacitance fibrous anodes is a major bottleneck to achieve high performance FALICs. Here, hierarchical MoS₂@α‐Fe₂O₃ core–shell heterostructures consisting of spindle‐shaped α‐Fe₂O₃ cores and MoS₂ nanosheet shells on a carbon nanotube fiber (CNTF) are successfully fabricated. Originating from the unique core/shell architecture and prominent synergetic effects for multi‐components, the resulting MoS₂@α‐Fe₂O₃/CNTF anode delivers a remarkable specific capacitance of 2077.5 mF cm^?2 (554.0 F cm^?3) at 2 mA cm^?2, substantially outperforming most of the previously reported fibrous anode materials. Further density functional theory calculations reveal that the MoS₂@α‐Fe₂O₃ nano‐heterostructure possesses better electrical conductivity and stronger adsorption energy of Li⁺ than those of the individual MoS₂ and α‐Fe₂O₃. By paring with the self‐standing LiCoO₂/CNTF battery‐type cathode, a prototype quasi‐solid‐state FALIC with a maximum operating voltage of 2.0 V is constructed, achieving impressive specific capacitance (253.1 mF cm^?2) and admirable energy density (39.6 mWh cm^?3). Additionally, the newly developed FALICs can be woven into the flexible textile to power wearable electronics. This work presents a novel effective strategy to design high‐performance anode materials for next‐generation wearable ALICs.     

Multifunctional Self-Charging Electrochromic Supercapacitors Driven by Direct-Current Triboelectric Nanogenerators

Electrochromic supercapacitor devices (ESCDs) are highly promising for energy-saving applications or smart windows, whereas they still require electrical energy inputs. In this study, a self-charging ESCD (SC-ESCD) based on the ESCD and a sliding-mode direct-current triboelectric nanogenerators is successfully proposed. The SC-ESCD cannot merely convert mechanical sliding kinetic energy into electrical energy and store the electricity in electrochromic supercapacitors but can also show optical responses to the mechanical sliding motions. The prominent electrochemical performances of the SC-ESCD are confirmed by the high areal capacitance (15.2 mF cm⁻² at 0.1 mA cm⁻²) and stable cycling performance (99% for 5000 cycles). Besides, it can be prepared into arbitrary characters or patterns to adapt to various applications. The study demonstrates a potential approach to develop multifunctional self-charging power sources which combine energy harvesting, energy storage, and electrochromic functions.     

Uniform Virus‐Like Co–N–Cs Electrocatalyst Derived from Prussian Blue Analog for Stretchable Fiber‐Shaped Zn–Air Batteries

Zn‐air batteries (ZABs) offer promising commercialization perspectives for stretchable and wearable electronic devices as they are environment‐friendly and have high theoretical energy density. However, current devices suffer from limited energy efficiency and durability because of the sluggish oxygen reduction and evolution reactions kinetics in the air cathode as well as degenerative stretchability of solid‐state electrolytes under highly alkaline conditions. Herein, excellent bifunctional catalytic activity and cycling stability is achieved by using a newly developed Co–N–C nanomaterial with a uniform virus‐like structure, prepared via a facile carbonization of a prussian blue analogue (PBA). Furthermore, a solid‐state dual‐network sodium polyacrylate and cellulose (PANa‐cellulose) based hydrogel electrolyte is synthesized with good alkaline‐tolerant stretchability. A solid‐state fiber‐shaped ZAB fabricated using this hydrogel electrolyte, the virus‐like Co–N–Cs air cathode, and a zinc spring anode display excellent stretchability of up to 500% strain without damage, and outstanding electrochemical performance with 128 mW cm^?2 peak power density and good cycling stability for >600 cycles at 2 mA. The facile synthesis strategy demonstrated here opens up a new avenue for developing highly active PBA‐derived catalyst and shows, for the first time, that virus‐like structure can be favorable for electrochemical performance.     

General Method for Large‐Area Films of Carbon Nanomaterials and Application of a Self‐Assembled Carbon Nanotube Film as a High‐Performance Electrode Material for an All‐Solid‐State Supercapacitor

Rational assembly of carbon nanostructures into large‐area films is a key step to realize their applications in ubiquitous electronics and energy devices. Here, a self‐assembly methodology is devised to organize diverse carbon nanostructures (nanotubes, dots, microspheres, etc.) into homogeneous films with potentially infinite lateral dimensions. On the basis of studies of the redox reactions in the systems and the structures of films, the spontaneous deposition of carbon nanostructures onto the surface of the copper substrate is found to be driven by the electrical double layer between copper and solution. As a notable example, the as‐assembled multiwalled carbon nanotube (MWCNT) films display exceptional properties. They are a promising material for flexible electronics with superior electrical and mechanical compliance characteristics. Finally, two kinds of all‐solid‐state supercapacitors based on the self‐assembled MWCNT films are fabricated. The supercapacitor using carbon cloth as the current collector delivers an energy density of 3.5 Wh kg^?1 and a power density of 28.1 kW kg^?1, which are comparable with the state‐of‐the‐art supercapacitors fabricated by the costly single‐walled carbon nanotubes and arrays. The supercapacitor free of foreign current collector is ultrathin and shows impressive volumetric energy density (0.58 mWh cm^?3) and power density (0.39 W cm^?3) too.     

A Low‐Cost,Self‐Standing NiCo2O4@CNT/CNT Multilayer Electrode for Flexible Asymmetric Solid‐State Supercapacitors

The demand for a new generation of flexible, portable, and high‐capacity power sources increases rapidly with the development of advanced wearable electronic devices. Here we report a simple process for large‐scale fabrication of self‐standing composite film electrodes composed of NiCo₂O₄@carbon nanotube (CNT) for supercapacitors. Among all composite electrodes prepared, the one fired in air displays the best electrochemical behavior, achieving a specific capacitance of 1,590 F g^?1 at 0.5 A g^?1 while maintaining excellent stability. The NiCo₂O₄@CNT/CNT film electrodes are fabricated via stacking NiCo₂O₄@CNT and CNT alternately through vacuum filtration. Lightweight, flexible, and self‐standing film electrodes (≈24.3 µm thick) exhibit high volumetric capacitance of 873 F cm^?3 (with an areal mass of 2.5 mg cm^?2) at 0.5 A g^?1. An all‐solid‐state asymmetric supercapacitor consists of a composite film electrode and a treated carbon cloth electrode has not only high energy density (≈27.6 Wh kg^?1) at 0.55 kW kg^?1 (including the weight of the two electrodes) but also excellent cycling stability (retaining ≈95% of the initial capacitance after 5000 cycles), demonstrating the potential for practical application in wearable devices.     

Wearable Biofuel Cells: Advances from Fabrication to Application

The booming field of wearable devices has nourished progress in developing multifunctional wearable energy sources that can withstand deformations while maintaining their electrochemical functions. Unlike energy storage systems such as rechargeable batteries and supercapacitors, wearable biofuel cells (w-BFCs) generate green electricity from energy-dense carbon-neutral fuels via highly efficient bioelectrochemical reactions, delivering excellent biocompatibility, remarkable environmental sustainability, and exceptional capability of miniaturization. These desirable merits give w-BFCs great potential in the field of wearable applications. Moreover, emerging studies of w-BFCs in self-powered biosensing, controlled drug delivery, and wound dressings have greatly expanded their possible fields of application. Recent progress and strategies to accomplish flexible and stretchable w-BFCs are summarized here. Novel materials and configurations with tailored features that can be employed to fabricate w-BFCs are elaborated and discussed. Current applications and near-future applications of w-BFCs in health-monitoring and medical treatment fields are outlined. Furthermore, challenges and perspectives regarding this emerging field of materials science and engineering are also emphasized.     

Wearable and Implantable Triboelectric Nanogenerators

Triboelectric nanogenerators (TENGs) are a promising technology to convert mechanical energy to electrical energy based on coupled triboelectrification and electrostatic induction. With the rapid development of functional materials and manufacturing techniques, wearable and implantable TENGs have evolved into playing important roles in clinic and daily life from in vitro to in vivo. These flexible and light membrane‐like devices have the potential to be a new power supply or sensor element, to meet the special requirements for portable electronics, promoting innovation in electronic devices. In this review, the recent advances in wearable and implantable TENGs as sustainable power sources or self‐powered sensors are reviewed. In addition, the remaining challenges and future possible improvements of wearable and implantable TENG‐based self‐powered systems are discussed.     

Recent Progress in Solid Electrolytes for Energy Storage Devices

With the rapid advances in safe, flexible, and even stretchable electronic products, it is important to develop matching energy storage devices to more effectively power them. However, the use of conventional liquid electrolytes produces volatilization and leakage that are dangerous and requires strict packaging layers that are typically rigid. To this end, solid electrolytes that can overcome these problems have attracted increasing attention in recent decades. In this review article, three main types of solid electrolytes (i.e., inorganic, polymer, and composite electrolytes) are first described and compared in terms of their structures and properties. The advantages of solid electrolytes to make safe, flexible, stretchable, wearable, and self‐healing energy storage devices, including supercapacitors and batteries, are then discussed. The remaining challenges and possible directions are finally summarized to highlight future development in this field.