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

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

Flexible Zinc‐Ion Hybrid Fiber Capacitors with Ultrahigh Energy Density and Long Cycling Life for Wearable Electronics

Emerging wearable electronics require flexible energy storage devices with high volumetric energy and power densities. Fiber‐shaped capacitors (FCs) offer high power densities and excellent flexibility but low energy densities. Zn‐ion capacitors have high energy density and other advantages, such as low cost, nontoxicity, reversible Faradaic reaction, and broad operating voltage windows. However, Zn‐ion capacitors have not been applied in wearable electronics due to the use of liquid electrolytes. Here, the first quasisolid‐state Zn‐ion hybrid FC (ZnFC) based on three rationally designed components is demonstrated. First, hydrothermally assembled high surface area and conductive reduced graphene oxide/carbon nanotube composite fibers serve as capacitor‐type positive electrodes. Second, graphite fibers coated with a uniform Zn layer work as battery‐type negative electrodes. Third, a new neutral ZnSO₄‐filled polyacrylic acid hydrogel act as the quasisolid‐state electrolyte, which offers high ionic conductivity and excellent stretchability. The assembled ZnFC delivers a high energy density of 48.5 mWh cm^?3 at a power density of 179.9 mW cm^?3. Further, Zn dendrite formation that commonly happens under high current density is efficiently suppressed on the fiber electrode, leading to superior cycling stability. Multiple ZnFCs are integrated as flexible energy storage units to power wearable devices under different deformation conditions.     

Fully Bioabsorbable Natural‐Materials‐Based Triboelectric Nanogenerators

Implantable medical devices provide an effective therapeutic approach for neurological and cardiovascular diseases. With the development of transient electronics, a new power source with biocompatibility, controllability, and bioabsorbability becomes an urgent demand for medical sciences. Here, various fully bioabsorbable natural‐materials‐based triboelectric nanogenerators (BN‐TENGs), in vivo, are developed. The “triboelectric series” of five natural materials is first ranked, it provides a basic knowledge for materials selection and device design of the TENGs and other energy harvesters. Various triboelectric outputs of these natural materials are achieved by a single material and their pairwise combinations. The maximum voltage, current, and power density reach up to 55 V, 0.6 µA, and 21.6 mW m^?2, respectively. The modification of silk fibroin encapsulation film makes the operation time of the BN‐TENG tunable from days to weeks. After completing its function, the BN‐TENG can be fully degraded and resorbed in Sprague–Dawley rats, which avoids a second operation and other side effects. Using the proposed BN‐TENG as a voltage source, the beating rates of dysfunctional cardiomyocyte clusters are accelerated and the consistency of cell contraction is improved. This provides a new and valid solution to treat some heart diseases such as bradycardia and arrhythmia.     

Biodegradable Electronic Systems in 3D,Heterogeneously Integrated Formats

Biodegradable electronic systems represent an emerging class of technology with unique application possibilities, from temporary biomedical implants to “green” consumer gadgets. This paper introduces materials and processing methods for 3D, heterogeneously integrated devices of this type, with various functional examples in sophisticated forms of silicon‐based electronics. Specifically, techniques for performing multilayer assembly by transfer printing and for fabricating layer‐to‐layer vias and interconnects by lithographic procedures serve as routes to biodegradable, 3D integrated circuits composed of functional building blocks formed using specialized approaches or sourced from commercial semiconductor foundries. Demonstration examples range from logic gates and analog circuits that undergo functional transformation by transience to systems that integrate multilayer resistive sensors for in situ, continuous electrical monitoring of the processes of transience. The results significantly expand the scope of engineering options for biodegradable electronics and other types of transient microsystem technologies.     

Energy Harvesters for Wearable and Stretchable Electronics: From Flexibility to Stretchability

The rapid advancements of wearable electronics have caused a paradigm shift in consumer electronics, and the emerging development of stretchable electronics opens a new spectrum of applications for electronic systems. Playing a critical role as the power sources for independent electronic systems, energy harvesters with high flexibility or stretchability have been the focus of research efforts over the past decade. A large number of the flexible energy harvesters developed can only operate at very low strain level (≈0.1%), and their limited flexibility impedes their application in wearable or stretchable electronics. Here, the development of highly flexible and stretchable (stretchability >15% strain) energy harvesters is reviewed with emphasis on strategies of materials synthesis, device fabrication, and integration schemes for enhanced flexibility and stretchability. Due to their particular potential applications in wearable and stretchable electronics, energy‐harvesting devices based on piezoelectricity, triboelectricity, thermoelectricity, and dielectric elastomers have been largely developed and the progress is summarized. The challenges and opportunities of assembly and integration of energy harvesters into stretchable systems are also discussed.     

Atomically Thin Mesoporous Co3O4 Layers Strongly Coupled with N‐rGO Nanosheets as High‐Performance Bifunctional Catalysts for 1D Knittable Zinc–Air Batteries

Under development for next‐generation wearable electronics are flexible, knittable, and wearable energy‐storage devices with high energy density that can be integrated into textiles. Herein, knittable fiber‐shaped zinc–air batteries with high volumetric energy density (36.1 mWh cm^?3) are fabricated via a facile and continuous method with low‐cost materials. Furthermore, a high‐yield method is developed to prepare the key component of the fiber‐shaped zinc–air battery, i.e., a bifunctional catalyst composed of atomically thin layer‐by‐layer mesoporous Co₃O₄/nitrogen‐doped reduced graphene oxide (N‐rGO) nanosheets. Benefiting from the high surface area, mesoporous structure, and strong synergetic effect between the Co₃O₄ and N‐rGO nanosheets, the bifunctional catalyst exhibits high activity and superior durability for oxygen reduction and evolution reactions. Compared to a fiber‐shaped zinc–air battery using state‐of‐the‐art Pt/C + RuO₂ catalysts, the battery based on these Co₃O₄/N‐rGO nanosheets demonstrates enhanced and stable electrochemical performance, even under severe deformation. Such batteries, for the first time, can be successfully knitted into clothes without short circuits under external forces and can power various electronic devices and even charge a cellphone.     

MESFET Electronics: Recent Progress on ZnO‐Based Metal‐Semiconductor Field‐Effect Transistors and Their Application in Transparent Integrated Circuits (Adv. Mater. 47/2010)

Metal‐semiconductor field‐effect transistors (MESFETs) are widely known from opaque high‐speed GaAs or high‐power SiC and GaN technology. For the emerging field of transparent electronics, only metal‐insulator‐semiconductor field‐effect transistors (MISFETs) were considered so far. This article reviews the progress of high‐performance MESFETs in oxide electronics and reflects the recent advances of this technique towards transparent MESFET circuitry. We discuss design prospects as well as limitations regarding device performance, reliability and stability. The presented ZnO‐based MESFETs and inverters have superior properties compared to MISFETs, i.e., high channel mobilities and on/off‐ratios, high gain, and low uncertainty level at comparatively low operating voltages. This makes them a promising approach for future low‐cost transparent electronics.     

Materials,Processes, and Facile Manufacturing for Bioresorbable Electronics: A Review

Bioresorbable electronics refer to a new class of advanced electronics that can completely dissolve or disintegrate with environmentally and biologically benign byproducts in water and biofluids. They have provided a solution to the growing electronic waste problem with applications in temporary usage of electronics such as implantable devices and environmental sensors. Bioresorbable materials such as biodegradable polymers, dissolvable conductors, semiconductors, and dielectrics are extensively studied, enabling massive progress of bioresorbable electronic devices. Processing and patterning of these materials are predominantly relying on vacuum‐based fabrication methods so far. However, for the purpose of commercialization, nonvacuum, low‐cost, and facile manufacturing/printing approaches are the need of the hour. Bioresorbable electronic materials are generally more chemically reactive than conventional electronic materials, which require particular attention in developing the low‐cost manufacturing processes in ambient environment. This review focuses on material reactivity, ink availability, printability, and process compatibility for facile manufacturing of bioresorbable electronics.     

High‐Performance Two‐Ply Yarn Supercapacitors Based on Carbon Nanotube Yarns Dotted with Co3O4 and NiO Nanoparticles

Yarn supercapacitors are promising power sources for flexible electronic applications that require conventional fabric‐like durability and wearer comfort. Carbon nanotube (CNT) yarn is an attractive choice for constructing yarn supercapacitors used in wearable textiles because of its high strength and flexibility. However, low capacitance and energy density limits the use of pure CNT yarn in wearable high‐energy density devices. Here, transitional metal oxide pseudocapacitive materials NiO and Co₃O₄ are deposited on as‐spun CNT yarn surface using a simple electrodeposition process. The Co₃O₄ deposited on the CNT yarn surface forms a uniform hybridized CNT@Co₃O₄ layer. The two‐ply supercapacitors formed from the CNT@Co₃O₄ composite yarns display excellent electrochemical properties with very high capacitance of 52.6 mF cm^?2 and energy density of 1.10 μWh cm^?2. The high performance two‐ply CNT@Co₃O₄ yarn supercapacitors are mechanically and electrochemically robust to meet the high performance requirements of power sources for wearable electronics.     

Buckled Structures: Fabrication and Applications in Wearable Electronics

Wearable electronics have attracted a tremendous amount of attention due to their many potential applications, such as personalized health monitoring, motion detection, and smart clothing, where electronic devices must conformably form contacts with curvilinear surfaces and undergo large deformations. Structural design and material selection have been the key factors for the development of wearable electronics in the recent decades. As one of the most widely used geometries, buckling structures endow high stretchability, high mechanical durability, and comfortable contact for human–machine interaction via wearable devices. In addition, buckling structures that are derived from natural biosurfaces have high potential for use in cost‐effective and high‐grade wearable electronics. This review provides fundamental insights into buckling fabrication and discusses recent advancements for practical applications of buckled electronics, such as interconnects, sensors, transistors, energy storage, and conversion devices. In addition to the incorporation of desired functions, the simple and consecutive manipulation and advanced structural design of the buckled structures are discussed, which are important for advancing the field of wearable electronics. The remaining challenges and future perspectives for buckled electronics are briefly discussed in the final section.     

Recent Progress in Rechargeable Sodium‐Ion Batteries: toward High‐Power Applications

The increasing demands for renewable energy to substitute traditional fossil fuels and related large‐scale energy storage systems (EES) drive developments in battery technology and applications today. The lithium‐ion battery (LIB), the trendsetter of rechargeable batteries, has dominated the market for portable electronics and electric vehicles and is seeking a participant opportunity in the grid‐scale battery market. However, there has been a growing concern regarding the cost and resource availability of lithium. The sodium‐ion battery (SIB) is regarded as an ideal battery choice for grid‐scale EES owing to its similar electrochemistry to the LIB and the crust abundance of Na resources. Because of the participation in frequency regulation, high pulse‐power capability is essential for the implanted SIBs in EES. Herein, a comprehensive overview of the recent advances in the exploration of high‐power cathode and anode materials for SIB is presented, and deep understanding of the inherent host structure, sodium storage mechanism, Na⁺ diffusion kinetics, together with promising strategies to promote the rate performance is provided. This work may shed light on the classification and screening of alternative high rate electrode materials and provide guidance for the design and application of high power SIBs in the future.     

A Quasi‐Solid‐State Flexible Fiber‐Shaped Li–CO2 Battery with Low Overpotential and High Energy Efficiency

The rapid development of wearable electronics requires a revolution of power accessories regarding flexibility and energy density. The Li–CO₂ battery was recently proposed as a novel and promising candidate for next‐generation energy‐storage systems. However, the current Li–CO₂ batteries usually suffer from the difficulties of poor stability, low energy efficiency, and leakage of liquid electrolyte, and few flexible Li–CO₂ batteries for wearable electronics have been reported so far. Herein, a quasi‐solid‐state flexible fiber‐shaped Li–CO₂ battery with low overpotential and high energy efficiency, by employing ultrafine Mo₂C nanoparticles anchored on a carbon nanotube (CNT) cloth freestanding hybrid film as the cathode, is demonstrated. Due to the synergistic effects of the CNT substrate and Mo₂C catalyst, it achieves a low charge potential below 3.4 V, a high energy efficiency of ≈80%, and can be reversibly discharged and charged for 40 cycles. Experimental results and theoretical simulation show that the intermediate discharge product Li₂C₂O₄ stabilized by Mo₂C via coordinative electrons transfer should be responsible for the reduction of overpotential. The as‐fabricated quasi‐solid‐state flexible fiber‐shaped Li–CO₂ battery can also keep working normally even under various deformation conditions, giving it great potential of becoming an advanced energy accessory for wearable electronics.     

A Colloidal‐Quantum‐Dot‐Based Self‐Charging System via the Near‐Infrared Band

A novel self‐charging platform is proposed using colloidal‐quantum‐dot (CQD) photovoltaics (PVs) via the near‐infrared (NIR) band for low‐power electronics. Low‐bandgap CQDs can convert invisible NIR light sources to electrical energy more efficiently than wider spectra because of reduced thermalization loss. This energy‐conversion strategy via NIR photons ensures an enhanced photostability of the CQD devices. Furthermore, the NIR wireless charging system can be concealed using various colored and NIR‐transparent fabric or films, providing aesthetic freedom. Finally, an NIR‐driven wireless charging system is demonstrated for a wearable healthcare bracelet by integrating a CQD PVs receiver with a flexible lithium‐ion battery and entirely embedding them into a flexible strap, enabling permanent self‐charging without detachment.     

Flexible 1D Batteries: Recent Progress and Prospects

With the rapid development of wearable and portable electronics, flexible and stretchable energy storage devices to power them are rapidly emerging. Among numerous flexible energy storage technologies, flexible batteries are considered as the most favorable candidate due to their high energy density and long cycle life. In particular, flexible 1D batteries with the unique advantages of miniaturization, adaptability, and weavability are expected to be a part of such applications. The development of 1D batteries, including lithium-ion batteries, zinc-ion batteries, zinc–air batteries, and lithium–air batteries, is comprehensively summarized, with particular emphasis on electrode preparation, battery design, and battery properties. In addition, the remaining challenges to the commercialization of current 1D batteries and prospective opportunities in the field are discussed.     

Physically Transient Threshold Switching Device Based on Magnesium Oxide for Security Application

Transient memristors are prospective candidates for both secure memory systems and biointegrated electronics, which are capable to physically disappear at a programmed time with a triggered operation. However, the sneak current issue has been a considerable obstacle to achieve high‐density transient crossbar array of memristors. To solve this problem, it is necessary to develop a transient switch device to turn the memory device on and off controllably. Here, a dissolvable and flexible threshold switching (TS) device with a vertically crossed structure is introduced, which exhibits a high selectivity of 10⁷, steep turn‐on slope of <8 mV dec⁻¹, and fast ON/OFF switch speed within 50/25 ns. Triggered failure could be achieved after soaking the device in deionized water for 8 min at room temperature. Furthermore, a water‐assisted transfer printing method is used to fabricate flexible and transient TS device arrays for bioresorbable systems, in which none of any significant degradation is observed under a bending radius of 2 mm. Integrating the selector with a transient memristor is capable of 10⁷ Gb memory implementation, indicating that the transient TS device could provide great opportunities to achieve highly integrated transient memory arrays.     

An All‐Stretchable‐Component Sodium‐Ion Full Battery

Stretchable energy‐storage devices receive considerable attention due to their promising applications in future wearable technologies. However, they currently suffer from many problems, including low utility of active materials, limited multidirectional stretchability, and poor stability under stretched conditions. In addition, most proposed designs use one or more rigid components that fail to meet the stretchability requirement for the entire device. Here, an all‐stretchable‐component sodium‐ion full battery based on graphene‐modified poly(dimethylsiloxane) sponge electrodes and an elastic gel membrane is developed for the first time. The battery exhibits reasonable electrochemical performance and robust mechanical deformability; its electrochemical characteristics can be well‐maintained under many different stretched conditions and after hundreds of stretching–release cycles. This novel design integrating all stretchable components provides a pathway toward the next generation of wearable energy devices in modern electronics.     

Stretchable,Large‐area Organic Electronics

Stretchability will significantly expand the application scope of electronics, particularly large‐area electronics—displays, sensors, and actuators. If arbitrary surfaces and movable parts could be covered with stretchable electronics, which is impossible with conventional electronics, new classes of applications are expected to emerge. A large hurdle is manufacturing electrical wiring with high conductivity, high stretchability, and large‐area compatibility. This Review describes stretchable, large‐area electronics based on organic field‐effect transistors for applications to sensors and displays. First, novel net‐shaped organic transistors are employed to realize stretchable, large‐area sensor networks that detect distributions of pressure and temperature simultaneously. The whole system is functional even when it is stretched by 25%. In order to further improve stretchability, printable elastic conductors are developed by dispersing single‐walled carbon nanotubes (SWNTs) as dopants uniformly in rubbers. Further, we describe integration of printable elastic conductors with organic transistors to construct a rubber‐like stretchable active matrix for large‐area sensor and display applications. Finally, we will discuss the future prospects of stretchable, large‐area electronics with delineating a picture of the next‐generation human/machine interfaces from the aspect of materials science and electronic engineering.     

The Design of 3D‐Interface Architecture in an Ultralow‐Power,Electrospun Single‐Fiber Synaptic Transistor for Neuromorphic Computing

Synaptic electronics is a new technology for developing functional electronic devices that can mimic the structure and functions of biological counterparts. It has broad application prospects in wearable computing chips, human–machine interfaces, and neuron prostheses. These types of applications require synaptic devices with ultralow energy consumption as the effective energy supply for wearable electronics, which is still very difficult. Here, artificial synapse emulation is demonstrated by solid‐ion gated organic field‐effect transistors (OFETs) with a 3D‐interface conducting channel for ultralow‐power synaptic simulation. The basic features of the artificial synapse, excitatory postsynaptic current (EPSC), paired‐pulse facilitation (PPF), and high‐pass filtering, are successfully realized. Furthermore, the single‐fiber based artificial synapse can be operated by an ultralow presynaptic spike down to ?0.5 mV with an ultralow reading voltage at ?0.1 mV due to the large contact surface between the ionic electrolyte and fiber‐like semiconducting channel. Therefore, the ultralow energy consumption at one spike of the artificial synapse can be realized as low as ≈3.9 fJ, which provides great potential in a low‐power integrated synaptic circuit.     

Toward Wearable Self‐Charging Power Systems: The Integration of Energy‐Harvesting and Storage Devices

One major challenge for wearable electronics is that the state‐of‐the‐art batteries are inadequate to provide sufficient energy for long‐term operations, leading to inconvenient battery replacement or frequent recharging. Other than the pursuit of high energy density of secondary batteries, an alternative approach recently drawing intensive attention from the research community, is to integrate energy‐generation and energy‐storage devices into self‐charging power systems (SCPSs), so that the scavenged energy can be simultaneously stored for sustainable power supply. This paper reviews recent developments in SCPSs with the integration of various energy‐harvesting devices (including piezoelectric nanogenerators, triboelectric nanogenerators, solar cells, and thermoelectric nanogenerators) and energy‐storage devices, such as batteries and supercapacitors. SCPSs with multiple energy‐harvesting devices are also included. Emphasis is placed on integrated flexible or wearable SCPSs. Remaining challenges and perspectives are also examined to suggest how to bring the appealing SCPSs into practical applications in the near future.     

Thermally drawn rechargeable battery fiber enables pervasive power

The increasing demand for mobile computing, communications, and robotics presents a growing need for suitable portable power solutions in non-flat customized electronic devices. Fibers as fundamental building blocks of fabrics and 3D-printed objects provide unique opportunities for developing pervasive multidimensional power systems. The characteristic small diameter (<10⁻³ m) and high aspect ratios (>10⁶) of fibers and expansion of fibers into 2D and 3D power systems necessitate ultra-long lengths to meet the energy specifications of portable electronic systems. Here, we present a Li-ion battery fiber, fabricated for the first time using a thermal drawing method which occurs with simultaneous flows of multiple complex electroactive gels, particles, and polymers within protective flexible cladding. This top-down approach allows for the production of fully-functional and arbitrarily long lithium-ion fiber batteries. The continuous 140 m fiber battery demonstrates a discharge capacity of ∼123 mAh and discharge energy of ∼217 mWh. The scalability and material tunability of these fibers position them for use in varied non-planar electronic systems, including a 1D-flexible electronic fiber, a 2D-large-scale machine woven electronic fabric (∼1.6 m²), and a 3D-printed structural electronic system. The fiber battery satisfies the requirements of portable electronics systems as it is machine washable, flexible, usable underwater, and fire/rupture-safe. We have demonstrated the powering of a submarine drone, LiFi fabric, and flying drone communication through different rechargeable fiber battery schemes, which paves the way for the emergence of the pervasive battery-powered electronics.