Highly Stretchable,Sparse, Metallized Nanofiber Webs as Thin,Transferrable Transparent Conductors

The need for transparent conductors (TCs) that are capable of withstanding high mechanical deformation in comparison to the brittle indium tin oxide (ITO) films is paramount for roll‐to‐roll production of flexible and stretchable displays, signage systems, lighting devices and solar panels with stringent weatherability requirements. This paper reports a highly stretchable TC comprising of a web of core‐shell nanofibers, which mimics the fibrous structure of natural systems such as veins of a leaf or nerve systems. The TC web demonstrates high transparency, low sheet resistance, and unprecedented stretchability and stability over repeated stretching. The nanofiber TC web can be transferred to different substrates, which is manifested by the transfer onto an organic solar cell, demonstrating a photovoltaic performance comparable to that of a device with an ITO electrode. This work presents a technological platform, scalable for the manufacturing of large area transparent conductors for flexible and stretchable displays, electronics and solar cells on unconventional substrates such as rubber, fabric and paper.     

A Stretchable Nanogenerator with Electric/Light Dual‐Mode Energy Conversion

As an alternative technology, stretchable electronics attract long‐lasting attention. A newly‐designed stretchable nanogenerator with unique dual‐mode energy conversion is reported. The ability of converting the input mechanical stimuli to either electric or light output is achieved by monolithically integrating a transparent single‐electrode triboelectric nanogenerator (S‐TENG) with a ZnS based mechanoluminescence (ML) composite. This stretchable device with versatile functions promotes the development of the smart systems to efficiently and diversely utilize ubiquitous mechanical energy and demonstrates great potential for artificial e‐skins.     

Enabling Deformable and Stretchable Batteries

Deformable energy storage devices are needed to power next‐generation wearable electronics that interface intimately with human skin. Currently, deformable energy storage devices demonstrate poor performance compared to their rigid lithium‐ion counterparts, forcing wearable manufacturers to design their devices around bulky battery compartments. However, technological advances to create deformable batteries at the component and device level have yielded continuous improvement in stretchable batteries over the last five years. In this Essay, the major strategies at the component and device level that have been successfully employed to create stretchable batteries are reviewed. The outstanding challenges facing deformable energy storage are also discussed, namely, energy density, packaging, delamination, device integration, and manufacturing. This Essay will give researchers who are interested in contributing to the development of deformable batteries a cursory understanding of the most successful strategies to date, and provide insights into the most important directions to pursue in the future.     

Enhancing Energy Storage Devices with Biomacromolecules in Hybrid Electrodes

The development of energy storage devices with higher energy and power outputs, and long cycling stability is urgently required in the pursuit of the expanding challenges of electrical energy storage. The utilization of biologically renewable redox compounds holds a great potential in designing sustainable energy storage systems and contributes in reducing the dependence on fossil fuels for energy materials. Quinones are the principal redox centers in natural organic materials and play a key role as charge storage electrode materials because of their abundance, multiple forms and integration into the materials flow through the biosphere. Electrical energy storage devices and systems can be significantly improved by the combination of scalable quinone‐based biomaterials with good electronic conductors. This review uses recent examples to show how biopolymers are providing new directions in the development of renewable biohybrid electrodes for energy storage devices.     

Stretchable Lithium‐Ion Batteries Enabled by Device‐Scaled Wavy Structure and Elastic‐Sticky Separator

Fast developments and substantial achievements have been shaping the field of wearable electronic devices, resulting in the persistent requirement for stretchable lithium‐ion batteries (LIBs). Despite recent progress in stretchable electrodes, stretching full batteries, including electrodes, separator, and sealing material, remains a great challenge. Here, a simple design concept for stretchable LIBs via a wavy structure at the full battery device scale is reported. All components including the package are capable of being reversibly stretched by folding the entire pouch cell into a wavy shape with polydimethylsiloxane filled in each valley region. In addition, the stretchable, sticky, and porous polyurethane/poly(vinylidene fluoride) membrane is adopted as a separator for the first time, which can maintain intimate contact between electrodes and separator to continuously secure ion pathway under dynamic state. Commercial cathode, anode, and package can be utilized in this rationally designed wavy battery to enable stretchability. The results indicate good electrochemical performances and long‐term stability at repeatable release–stretch cycles. A high areal capacity of 3.6 mA h cm^?2 and energy density of up to 172 W h L^?1 can be achieved for the wavy battery. The promising results of the cost‐effective wavy battery with high stretchability shed light on the development of stretchable energy storages.     

Design Considerations for Unconventional Electrochemical Energy Storage Architectures

Batteries have become fundamental building blocks for the mobility of modern society. Continuous development of novel battery chemistries and electrode materials has nourished progress in building better batteries. Simultaneously, novel device form factors and designs with multi‐functional components have been proposed, requiring batteries to not only integrate seamlessly to these devices, but to also be a multi‐functional component for a multitude of applications. Thus, in the past decade, along with developments in the component materials, the focus has been shifting more and more towards novel fabrication processes, unconventional configurations, and additional functionalities. This work attempts to critically review the developments with respect to emerging electrochemical energy storage configurations, including, amongst others, paintable, transparent, flexible, wire or cable shaped, ultra‐thin and ultra‐thick configurations, as well as hybrid energy storage‐conversion, or graphene‐incorporated batteries and supercapacitors. The performance requirements are elaborated together with the advantages, but also the limitations, with respect to established electrochemical energy storage technologies. Finally, challenges in developing novel materials with tailored properties that would allow such configurations, and in designing easier manufacturing techniques that can be widely adopted are considered.     

Highly Stretchable Supercapacitors via Crumpled Vertically Aligned Carbon Nanotube Forests

Stretchable supercapacitors have received increasing attention due to their broad applications in developing self‐powered stretchable electronics for wearable electronics, epidermal and implantable electronics, and biomedical devices that are capable of sustaining large deformations and conforming to complicated surfaces. In this work, a new type of highly stretchable and reliable supercapacitor is developed based on crumpled vertically aligned carbon nanotube (CNT) forests transferred onto an elastomer substrate with the assistance of a thermal annealing process in atmosphere environment. The crumpled CNT‐forest electrodes demonstrated good electrochemical performance and stability under either uniaxial (300%) or biaxial strains (300% × 300%) for thousands of stretching–relaxing cycles. The resulting supercapacitors can sustain a stretchability of 800% and possess a specific capacitance of 5 mF cm^?2 at the scan rate of 50 mV s^?1. Furthermore, the crumpled CNT‐forest electrodes can be easily decorated with impregnated metal oxide nanoparticles to improve the specific capacitance and energy density of the supercapacitors. The approach developed in this work offers an alternative strategy for developing novel stretchable energy devices with vertically aligned nanotubes or nanowires for advanced applications in stretchable, flexible, and wearable electronic systems.     

Lithium Fast‐Ionic Conduction in Complex Hydrides: Review and Prospects

Complex hydrides exhibit various energy‐related functions such as hydrogen storage, microwave absorption, and neutron shielding. Furthermore, another novel energy‐related function was recently reported by the authors; lithium fast‐ionic conduction, which suggests that complex hydrides may be a potential candidate for solid electrolytes in lithium‐ion batteries. This review presents the recent progress in the development of lithium fast‐ionic conductors of complex hydrides. First, the fast‐ionic conduction in LiBH₄ as a result of clarifying the mechanism of microwave absorption is presented, and then the conceptual development of complex hydrides as a new type of solid‐state lithium fast‐ionic conductors in LiBH₄–, LiNH₂–, and LiAlH₄‐based complex hydrides is discussed. Finally, the future prospects of this study from both application and fundamental viewpoints are described: possible use as solid electrolytes for batteries, formation of ionic liquids in complex hydrides, and similarity between complex hydrides and Laves‐phase metal hydrides.     

Highly Stretchable Separator Membrane for Deformable Energy‐Storage Devices

With the emergence of stretchable electronic devices, there is growing interest in the development of deformable power accessories that can power them. To date, various approaches have been reported for replacing rigid components of typical batteries with elastic materials. Little attention, however, has been paid to stretchable separator membranes that can not only prevent internal short circuit but also provide an ionic conducting pathway between electrodes under extreme physical deformation. Herein, a poly(styrene‐b‐butadiene‐b‐styrene) (SBS) block copolymer–based stretchable separator membrane is fabricated by the nonsolvent‐induced phase separation (NIPS). The diversity of mechanical properties and porous structures can be obtained by using different polymer concentrations and tuning the affinity among major components of NIPS. The stretchable separator membrane exhibits a high stretchability of around 270% strain and porous structure having porosity of 61%. Thus, its potential application as a stretchable separator membrane for deformable energy devices is demonstrated by applying to organic/aqueous electrolyte–based rechargeable lithium‐ion batteries. As a result, these batteries manifest good cycle life and stable capacity retention even under a stretching condition of 100%, without compromising the battery's performance.     

Mechanically Recoverable and Highly Efficient Perovskite Solar Cells: Investigation of Intrinsic Flexibility of Organic–Inorganic Perovskite

Highly efficient solar cells with sustainable performance under severe mechanical deformations are in great demand for future wearable power supply devices. In this regard, numerous studies have progressed to implement flexible architecture to high‐performance devices such as perovskite solar cells. However, the absence of suitable flexible and stretchable materials has been a great obstacle in the replacement of largely utilized transparent conducting oxides that are limited in flexibility. Here, a shape recoverable polymer, Noland Optical Adhesive 63, is utilized as a substrate of perovskite solar cell to enable complete shape recovery of the device upon sub‐millimeter bending radii. The employment of stretchable electrodes prevents mechanical damage of the perovskite layer. Before and after bending at a radius of 1 mm, power conversion efficiency (PCE) is measured to be 10.75% and 10.4%, respectively. Additionally, the shape recoverable device demonstrates a PCE of 6.07% after crumpling. The mechanical properties of all the layers are characterized by nanoindentation. Finite element analysis reveals that the outstanding flexibility of the perovskite layer enables small plastic strain distribution on the deformed device. These results clearly demonstrated that this device has great potential to be utilized in stretchable power supply applications.     

Stretchable Polymerized High Internal Phase Emulsion Separators for High Performance Soft Batteries

Powering soft embodiments of robots, machines and electronics is a key issue that impacts emerging human friendly forms of technologies. Batteries as energy source enable their untethered operation at high power density but must be rendered elastic to fully comply with (soft) robots and human beings. Current intrinsically stretchable batteries typically show decreased performance when deformed due to design limitations, mainly imposed by the separator material. High quality stretchable separators such as gel electrolytes represent a key component of soft batteries that affects power, internal resistance, and capacity independently of battery chemistry. Here, polymerized high internal phase emulsions (polyHIPEs) are introduced as highly ionically conductive separators in stretchable (rechargeable) batteries. Highly porous (>80%) separators result in electrolyte to polyHIPE conductivity ratios of below 2, while maintaining stretchability of ≈50% strain. The high stretchability, tunable porosity, and fast ion transport enable stretchable batteries with internal resistance below 3 Ω and 16.8 mAh cm^?2 capacity that power on‐skin processing and communication electronics. The battery/separator architecture is universally applicable to boost battery performance and represents a step towards autonomous operation of conformable electronic skins for healthcare, robotics, and consumers.     

Highly Stable Transparent Conductive Silver Grid/PEDOT:PSS Electrodes for Integrated Bifunctional Flexible Electrochromic Supercapacitors

Silver grids are attractive for replacing indium tin oxide as flexible transparent conductors. This work aims to improve the electrochemical stability of silver‐based transparent conductors. A silver grid/PEDOT:PSS hybrid film with high conductivity and excellent stability is successfully fabricated. Its functionality for flexible electrochromic applications is demonstrated by coating one layer of WO₃ nanoparticles on the silver grid/PEDOT:PSS hybrid film. This hybrid structure presents a large optical modulation of 81.9% at 633 nm, fast switching, and high coloration efficiency (124.5 cm² C^?1). More importantly, an excellent electrochemical cycling stability (sustaining 79.1% of their initial transmittance modulation after 1000 cycles) and remarkable mechanical flexibility (optical modulation decay of only 7.5% after 1200 compressive bending cycles) is achieved. A novel smart supercapacitor is presented that functions as a regular energy‐storage device and simultaneously monitors the level of stored energy by a rapid and reversible color variation even at high current charge/discharge conditions. The film sustains an optical modulation of 87.7% and a specific capacitance of 67.2% at 10 A g^?1 compared to their initial value at a current density of 1 A g^?1. The high‐performance silver grid/PEDOT:PSS hybrid transparent films exhibit promising features for various emerging flexible electronics and optoelectronic devices.     

Highly Flexible and Transparent Polyionic‐Skin Triboelectric Nanogenerator for Biomechanical Motion Harvesting

The advances of flexible electronics have raised demand for power sources with adaptability, flexibility, and multifunctionalities. Triboelectric nanogenerators are promising replacements for traditional batteries. Here, a highly soft skin‐like, transparent, and easily adaptable biomechanical energy harvester, based on a hybrid elastomer and with a polyionic hydrogel as the electrification layer and current collector, is developed. By harvesting the energy in human motion, the device generates an open‐circuit voltage of 70 V, a short‐circuit current density of 30.2 mA m^?2, and a maximum power density of 2.79 W m^?2 in a single‐electrode working mode. Further, it is demonstrated that the device can deliver power under bending, curling or by simple tapping when attached to human skin. In addition, the optimal counterpart of the polyionic layer with highest electronegativity difference is selected from a series of contact electrification materials based on a two‐electrode working mode, where a flexible device with the matching counterparts is investigated. Serving as ionic conductor and electrification layer, this polyionic material shows promising application in future development of self‐powered flexible electronics.     

Fabrication and Characterization of a Conformal Skin-like Electronic System for Quantitative,Cutaneous Wound Management

Recent advances in the development of electronic technologies and biomedical devices offer opportunities for non-invasive, quantitative assessment of cutaneous wound healing on the skin. Existing methods, however, still rely on visual inspections through various microscopic tools and devices that normally include high-cost, sophisticated systems and require well trained personnel for operation and data analysis. Here, we describe methods and protocols to fabricate a conformal, skin-like electronics system that enables conformal lamination to the skin surface near the wound tissues, which provides recording of high fidelity electrical signals such as skin temperature and thermal conductivity. The methods of device fabrication provide details of step-by-step preparation of the microelectronic system that is completely enclosed with elastomeric silicone materials to offer electrical isolation. The experimental study presents multifunctional, biocompatible, waterproof, reusable, and flexible/stretchable characteristics of the device for clinical applications. Protocols of clinical testing provide an overview and sequential process of cleaning, testing setup, system operation, and data acquisition with the skin-like electronics, gently mounted on hypersensitive, cutaneous wound and contralateral tissues on patients.     

Super‐Stretchable Zinc–Air Batteries Based on an Alkaline‐Tolerant Dual‐Network Hydrogel Electrolyte

Stretchable devices need elastic hydrogel electrolyte as an essential component, while most hydrogels will lose their stretchability after being incorporated with strong alkaline solution. This is why highly stretchable zinc–air batteries have never been reported so far. Herein, super‐stretchable, flat‐ (800% stretchable) and fiber‐shaped (500% stretchable) zinc–air batteries are first developed by designing an alkaline‐tolerant dual‐network hydrogel electrolyte. In the dual‐network hydrogel electrolyte, sodium polyacrylate (PANa) chains contribute to the formation of soft domains and the carboxyl groups neutralized by hydroxyls as well as cellulose as potassium hydroxide stabilizer are responsible for vastly enhanced alkaline tolerance. The obtained super‐stretchable, flat zinc–air battery exhibits a high power density of 108.6 mW?cm^?2, increasing to 210.5 mW?cm^?2 upon being 800% stretched. Similar phenomena are observed for the 500% stretchable fiber‐shaped batteries. The devices can maintain stable power output even after being heavily deformed benefiting from the highly soft, alkaline‐tolerant hydrogel electrolyte developed. A bendable battery‐display system and water proof weavable fiber zinc–air battery are also demonstrated. This work will facilitate the progress of using zinc–air battery powering flexible electronics and smart clothes. Moreover, the developed alkaline‐tolerant super‐stretchable electrolyte can also be applied for many other alkaline electrolyte‐based energy storage/conversion devices.     

Textile‐Based Electrochemical Energy Storage Devices

In the past few years, insensitive attentions have been drawn to wearable and flexible energy storage devices/systems along with the emergence of wearable electronics. Much progress has been achieved in developing flexible electrochemical energy storage devices with high end‐use performance. However, challenges still remain in well balancing the electrochemical properties, mechanical properties, and the processing technologies. In this review, a specific perspective on the development of textile‐based electrochemical energy storage devices (TEESDs), in which textile components and technologies are utilized to enhance the energy storage ability and mechanical properties of wearable electronic devices, is provided. The discussion focuses on the material preparation and characteristics, electrode and device fabrication strategies, electrochemical performance and metrics, wearable compatibility, and fabrication scalability of TEESDs including textile‐based supercapacitors and lithium‐ion batteries.     

Flexible and Semitransparent Organic Solar Cells

Flexible and semitransparent organic solar cells (OSCs) have been regarded as the most promising photovoltaic devices for the application of OSCs in wearable energy resources and building‐integrated photovoltaics. Therefore, the flexible and semitransparent OSCs have developed rapidly in recent years through the synergistic efforts in developing novel flexible bottom or top transparent electrodes, designing and synthesizing high performance photoactive layer and low temperature processed electrode buffer layer materials, and device architecture engineering. To date, the highest power conversion efficiencies have reached over 10% of the flexible OSCs and 7.7% with average visible transmittance of 37% for the semitransparent OSCs. Here, a comprehensive overview of recent research progresses and perspectives on the related materials and devices of the flexible and semitransparent OSCs is provided.     

A Stretchable Polymer–Carbon Nanotube Composite Electrode for Flexible Lithium‐Ion Batteries: Porosity Engineering by Controlled Phase Separation

Flexible energy‐storage devices have attracted growing attention with the fast development of bendable electronic systems. However, it still remains a challenge to find reliable electrode materials with both high mechanical flexibility/toughness and excellent electron and lithium‐ion conductivity. This paper reports the fabrication and characterization of highly porous, stretchable, and conductive polymer nanocomposites embedded with carbon nanotubes (CNTs) for application in flexible lithium‐ion batteries. The systematic optimization of the porous morphology is performed by controllably inducing the phase separation of polymethylmethacrylate (PMMA) in polydimethylsiloxane (PDMS) and removing PMMA, in order to generate well‐controlled pore networks. It is demonstrated that the porous CNT‐embedded PDMS nanocomposites are capable of good electrochemical performance with mechanical flexibility, suggesting these nanocomposites could be outstanding anode candidates for use in flexible lithium‐ion batteries. The optimization of the pore size and the volume fraction provides higher capacity by nearly seven‐fold compared to a nonporous nanocomposite.     

Computation‐Guided Design of LiTaSiO5, a New Lithium Ionic Conductor with Sphene Structure

The development of all‐solid‐state Li‐ion batteries requires solid electrolyte materials with many desired properties, such as ionic conductivity, chemical and electrochemical stability, and mechanical durability. Computation‐guided materials design techniques are advantageous in designing and identifying new solid electrolytes that can simultaneously meet these requirements. In this joint computational and experimental study, a new family of fast lithium ion conductors, namely, LiTaSiO₅ with sphene structure, are successfully identified, synthesized, and demonstrated using a novel computational design strategy. First‐principles computation predicts that Zr‐doped LiTaSiO₅ sphene materials have fast Li diffusion, good phase stability, and poor electronic conductivity, which are ideal for solid electrolytes. Experiments confirm that Zr‐doped LiTaSiO₅ sphene structure indeed exhibits encouraging ionic conductivity. The lithium diffusion mechanisms in this material are also investigated, indicating the sphene materials are 3D conductors with facile 1D diffusion along the [101] direction and additional cross‐channel migration. This study demonstrates a novel design strategy of activating fast Li ionic diffusion in lithium sphenes, a new materials family of superionic conductors.     

Programmable Nanocarbon‐Based Architectures for Flexible Supercapacitors

Supercapacitors (SCs), also called electrochemical capacitors, often show high power density, excellent charge/discharge rates, and long cycle life. The recent development of flexible and wearable electronic devices requires that their power sources be sufficiently compact and flexible to match these electronic components. Therefore, flexible SCs have attracted much attention to power current advanced electronics that can be flexible and wearable. In the past several years, many different strategies have been developed to programmably construct different nanocarbon materials into bendable electrode architectures. Furthermore, flexible SC devices with simplified configurations have also been designed based on these nanocarbon‐based architectures. Here, recent developments in the programmable assembly of bendable architectures based on nanocarbon materials are presented. Additionally, the design of flexible nanocarbon‐based SC devices with various configurations is highlighted. The progress made recently paves the way for further development of nanocarbon architectures and corresponding flexible SC devices. Future development and prospects in this area are also analyzed.