Construction of Flexible Piezoceramic Array with Ultrahigh Piezoelectricity via a Hierarchical Design Strategy

The µW-level power density of flexible piezoelectric energy harvesters (FPEHs) restricts their potential in applications related to high-power multifunctional wearable devices. To overcome this challenge, a hierarchical design strategy is proposed by forming porous piezoceramics with an optimum microstructure into an ordered macroscopic array structure to enable the construction of high performance FPEHs. The porous piezoceramic elements allows optimization of the sensing and harvesting Figure of merit, and the array structure causes a high level of effective strain under a mechanical load. The introduction of a network of polymer channels between the piezoceramic array also provides increased device flexibility, thereby allowing the device to attach and conform to the curved contours of the human body. The unique hierarchical piezoceramic array architecture exhibits superior flexibility, a high open circuit voltage (618 V), high short circuit current (188 µA), and ultrahigh power density (19.1 mW cm⁻²). This energy density value surpasses previously reported high-performance FPEHs. The ultrahigh power flexible harvesting can charge a 0.1 F supercapacitor at 2.5 Hz to power high-power electronic devices. Finally, the FPEH is employed in two novel applications related to fracture healing monitoring and self-powered wireless position tracking in extreme environments.     

Stretchable,Washable, and Ultrathin Triboelectric Nanogenerators as Skin-Like Highly Sensitive Self-Powered Haptic Sensors

Accompanying the boom in multifunctional wearable electronics, flexible, sustainable, and wearable power sources are facing great challenges. Here, a stretchable, washable, and ultrathin skin-inspired triboelectric nanogenerator (SI-TENG) to harvest human motion energy and act as a highly sensitive self-powered haptic sensor is reported. With the optimized material selections and structure design, the SI-TENG is bestowed with some merits, such as stretchability ( ≈ 800%), ultrathin ( ≈ 89 µ m), and light-weight ( ≈ 0.23 g), which conformally attach on human skin without disturbing its contact. A stretchable composite electrode, which is formed by homogenously intertwining silver nanowires (AgNWs) with thermoplastic polyurethane (TPU) nanofiber networks, is fabricated through synchronous electrospinning of TPU and electrospraying of AgNWs. Based on the triboelectrification effect, the open-circuit voltage, short-circuit current, and power density of the SI-TENG with a contact area of 2 × 2 cm² and an applied force of 8 N can reach 95 V, 0.3 µ A, and 6 mW m⁻², respectively. By integrating the signal-processing circuits, the SI-TENG with excellent energy harvesting and self-powered sensing capability is demonstrated as a haptic sensor array to detect human actions. The SI-TENG exhibits extensive applications in the fields of human–machine interface and security systems.     

A Textile-Based Temperature-Tolerant Stretchable Supercapacitor for Wearable Electronics

Among the extensive development of wearable electronics, which can be implanted onto bodies or embedded in clothes, textile-based devices have gained significant attention. For daily basis applications, wearable energy storage devices are required to be stable under harsh environmental conditions and different deformational conditions. In this study, a textile-based stretchable supercapacitor with high electrochemical performance, mechanical stability, and temperature tolerance over a wide temperature range is reported. It exhibits high areal capacitances of 28.0, 30.4, and 30.6 mF cm⁻² at −30, 25, and 80 °C, respectively, while the capacitance remains stable over three repeated cycles of cooling and heating from −30 to 80 °C. The supercapacitor is stable under stretching up to 50% and 1000 repetitive cycles of stretching. A temperature sensor and an liquid-crystal display are simultaneously driven at temperatures between −20 and 80 °C by the supercapacitors. The supercapacitors are woven into a nylon glove power a micro-light-emitting diode stably regardless of the bending of the index finger. Furthermore, the encapsulated supercapacitors retain the capacitance during being immersed in water for a few days. This study demonstrates the potential application of the fabricated supercapacitor as a wearable energy storage device that works under extreme temperature variations, high humidity, and body movements.     

Ultrahigh-Areal Capacitance Flexible Supercapacitors Based on Laser Assisted Construction of Hierarchical Aligned Carbon Nanotubes

Electrochemical energy storage is a key technology for a clean and sustainable energy supply. In this respect, supercapacitors (SC) have recently received considerable attention due to their excellent performance, including high-power density and long-cycle life. However, the poor binding strength between the active materials and substrate, the low active material loading, and small specific capacitance hinder the overall performance improvement of the device. In this study, an ultrahigh-areal capacitance flexible SC based on the Al micro grid-based hierarchical vertically aligned carbon nanotubes (VACNTs) is studied. Interestingly, the Al micro grid-based VACNTs exhibit ultrahigh loading (13 mg cm⁻²), and the as-fabricated VACNTs electrode display outstanding electrochemical performance, including an impressive areal capacitance of 1,300 mF cm⁻² at the current density of 13 mA cm⁻² and excellent stability with a retention ratio of 90% after 20,000 cycles at the current density of 130 mA cm⁻². Furthermore, the hierarchical VACNT electrodes show excellent mechanical flexibility when assembled into quasi-solid-state SC using Na₂SO₄-PVA gel as the electrolyte. The capacitance of this device is hardly changed bending different angles, even 180°. This study demonstrates the tremendous potential of Al micro grid-based hierarchical VACNTs as electrodes for high-performance flexible and wearable energy storage devices.     

Cellular Polypropylene Piezoelectret for Human Body Energy Harvesting and Health Monitoring

Self‐powered and wearable electronics, which are away from the problems of batteries, can provide the sustainable and comfortable interactive service for people. In this work, cellular polypropylene piezoelectret, which is with excellent physical and electrical properties, is utilized to build the human body energy harvesting and self‐powered human health monitoring systems. The cellular polypropylene piezoelectret flexible generator can reach a maximum peak power density of ≈52.8 mW m^?2. Simultaneously, self‐powered human body biological signals detecting sensors are demonstrated to detect the human physiological signals, such as coughing action and arterial pulses. This study strongly indicates the great compatibility and potential applications in human healthy monitoring may pave a new developing way for portable and wearable electronics systems.     

3D Printing-Directed Synergistic Design of High-Performance Zinc-Ion Hybrid Capacitors and Nanogenerators for All-In-One Self-Powered Energy Wristband

Advanced wearable self-powered energy systems that simultaneously achieve energy harvesting and energy storage offer exciting opportunities for flexible electronics, information communication, and even intelligent environmental monitoring. However, building and integrating synergistic energy storage from energy harvester unit into a single power source is highly challenging. Herein, a unique 3D printing-directed synergistic design of high-performance zinc-ion hybrid capacitors (ZIHCs) and triboelectric nanogenerators (TENGs) is proposed for the all-in-one self-powered wearable energy wristband. With advanced ink design, high-performance flexible ZIHCs are built up as the excellent energy storage unit with remarkable electrochemical behaviors and synergistic matching from TENGs. An exceptional device capacitance of 239.0 mF cm⁻², moderate potential window, high-rate capability, robust cycling stability, and excellent flexibility are achieved. Intrinsic charge storage process is also revealed, further demonstrating the outstanding electrochemical stability of the in-plane flexible ZIHCs. Moreover, using 3D printing-directed synergistic design, an advanced all-in-one self-powered energy wristband is developed, where an efficient harvesting of body vibration/movement energy and a reliable storage of harvested energy are simultaneously realized, representing a substantial step toward future practical applications in portable and wearable electronics.     

Stretchable and Flexible Buckypaper‐Based Lactate Biofuel Cell for Wearable Electronics

This work demonstrates a stretchable and flexible lactate/O₂ biofuel cell (BFC) using buckypaper (BP) composed of multi‐walled carbon nanotubes as the electrode material. Free‐standing BP, functionalized with a pyrene‐polynorbornene homopolymer, is fabricated as the immobilization matrix for lactate oxidase (LOx) at the anode and bilirubin oxidase at the cathode. This biofuel cell delivers an open circuit voltage of 0.74 V and a high‐power density of 520 µW cm^?2. The functionalized BP electrodes are assembled onto a stretchable screen‐printed current collector with an “island–bridge” configuration, which ensures conformal contact between the wearable BFC and the human body and endows the BFC with excellent performance stability under stretching condition. When applied to the arm of the volunteer, the BFC can generate a maximum power of 450 µW. When connected with a voltage booster, the on‐body BFC is able to power a light emitting diode under both pulse discharge and continuous discharge modes during exercise. This demonstrates the promising potential of the flexible BP‐based BFC as a self‐sustained power source for next‐generation wearable electronics.     

Body Heat Powered Wirelessly Wearable System for Real-time Physiological and Biochemical Monitoring

Through harvesting energy from the environment or human body, self-power wearable electronics have an opportunity to break through the limitations of battery supply and achieving long-term continuous operation. Here, a wireless wearable monitoring system driven entirely by body heat is implemented. Based on the principle of maximizing heat utilization, while optimizing internal resistance and heat dissipation, the stretchable TEG improves the power density of previous similar devices from only a few microwatts per square centimeter to tens and makes it possible to continuously drive wireless wearable electronic systems. Furthermore, ceaseless self-power energy gives wearable electronics unparalleled continuous working ability, which can realize the tracking and monitoring of biochemical and physiological indicators at different time scale. A practical system demonstrates the ability to real-time monitor heart rate, sweat ingredient and body motion at a high sampling rate. This study marks an important advance of self-powered wearable electronics for wirelessly real-time healthy monitoring.     

Flexible organic field-effect transistors based on electrospun conjugated polymer nanofibers with high bending stability

We report on flexible, single electrospun nanofiber field-effect transistors made by a blend of poly(3-decylthiophene) and poly(3-hexylthiophene), assessing for the first time the performances of this class of devices in terms of stability upon repeated tensile bending. Charge-carrier mobilities in the nanofiber-based device are estimated of the order of 10⁻³ cm²/(V s). Repeated cycles of bending and relaxing are performed, and the evolution of the device current–voltage characteristics is monitored up to 1000 cycles. We find that during bending the mobility is higher than that measured in planar conditions, and that after about 100 bending cycles it rapidly stabilizes. The here observed bending stability suggests a high compatibility of electrospun nanofibers with devices fabricated by roll-to-roll processes, and with bendable or wearable electronics.     

Surface Engineering of Carbon via Coupled Porosity Tuning and Heteroatom-Doping for High-Performance Flexible Fibrous Supercapacitors

Flexible fibrous supercapacitors (FFS) are considered the next-generation wearable energy storage devices because they provide reliable safety, eco-friendliness, and high power density. In particular, the FFS is desirable for application to wearable electronics because it can overcome disadvantages of the lithium-ion battery (LIB), such as the hazard of explosion and the complex manufacturing process. Nevertheless, the practical application of the FFS continues to be inhibited by the poor energy storage performance due to the limited specific surface area, poor electrical properties, and low wettability of the carbon fiber electrode. Herein, for the first time, the surface engineering of an FFS using nitrogen and fluorine codoped mesoporous carbon fibers (FFS-NFMCF) is described, and the synergistic effect of porosity tuning and heteroatom codoping upon the electrochemical performance is demonstrated. The resultant supercapacitor shows a high specific capacitance of 243.9 mF cm⁻² at a current density of 10.0 µA cm⁻² and good ultrafast cycling stability with capacitance retention of 91.3% for up to 10 000 cycles at a current density of 250.0 µA cm⁻². More interestingly, the FFS-NFMCF exhibits good mechanical properties and remarkable safety in practical application, thus demonstrating its feasibility for use in wearable electronic textiles.     

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.     

Flexible Sodium‐Ion Pseudocapacitors Based on 3D Na2Ti3O7 Nanosheet Arrays/Carbon Textiles Anodes

Flexible energy storage devices are critical components for emerging flexible and wearable electronics. Improving the electrochemical performance of flexible energy storage devices depends largely on development of novel electrode architectures and new systems. Here, a new class of flexible energy storage device called flexible sodium‐ion pseudocapacitors is developed based on 3D‐flexible Na₂Ti₃O₇ nanosheet arrays/carbon textiles (NTO/CT) as anode and flexible reduced graphene oxide film (GFs) as cathode without metal current collectors or conducting additives. The NTO/CT anode with advanced electrode architectures is fabricated by directly growing Na₂Ti₃O₇ nanosheet arrays on carbon textiles with robust adhesion through a simple hydrothermal process. The flexible GF//NTO/CT configuration achieves a high energy density of 55 Wh kg^?1 and high power density of 3000 W kg^?1. Taking the fully packaged flexible sodium‐ion pseudocapacitors into consideration, the maximum practical volumetric energy density and power density reach up to 1.3 mWh cm^?3 and 70 mW cm^?3, respectively. In addition, the flexible GF//NTO/CT device demonstrates a stable electrochemical performances with almost 100% capacitance retention under harsh mechanical deformation.     

A Fully Self-Healing and Highly Stretchable Liquid-Free Ionic Conductive Elastomer for Soft Ionotronics

Soft ionic conductors hold great potential for soft ionotronics, such as ionic skin, human–machine interface and soft luminescent device. However, most hydrogel and ionogel-based soft ionic conductors suffer from freezing, evaporation and liquid leakage problems, which limit their use in complex environments. Herein, a class of liquid-free ionic conductive elastomers (ICEs) is reported as an alternative soft ionic conductor in soft ionotronics. These liquid-free ICEs offer a combination of desirable properties, including extraordinary stretchability (up to 1913%), toughness (up to 1.08 MJ cm⁻³), Young's modulus (up to 0.67 MPa), rapid fully self-healing capability at room temperature, and good conductivity (up to 1.01 × 10⁻⁵ S cm⁻¹). The application of these ICEs is demonstrated by creating a wearable sensor that can detect and discriminate minimal deformations and human body movements, such as finger or elbow joint flexion, walking, running, etc. In addition, self-healing soft ionotronic devices are demonstrated to confront mechanical breakdown, such as an ionic skin and an alternating-current electroluminescent device that can reuse from damage. It is believed that these liquid-free ICEs hold great promises for applications in wearable devices and soft ionotronics.     

Large Cumulative Capacity Enabled by Regulating Lithium Plating with Metal–Organic Framework Layers on Porous Carbon Nanotube Scaffolds

The high specific capacity of lithium metal is ideal to meet the current demand in rechargeable batteries but lithium dendrites and irreversible volume expansions are major hurdles. 3D lithium host materials can alleviate these problems by lowering the current density with large surface areas and accommodating lithium metal in their pores. However, lithium dendrites are persistently observed because of sluggish lithium-ion diffusion through tortuous pores, resulting in clogging and thereby dendrite growth. Herein, layered metal–organic frameworks (MOFs) are deposited on carboxylated carbon nanotube (CNT) scaffolds via coordination bonding. The MOF layer on the outside of the CNT scaffold has augmented lithium insertion into the porous scaffolds (24 mAh cm⁻² at 8 mA cm⁻²) and lithium plating/stripping lifetime (over 1700 h with 20 mAh cm⁻² cycle⁻¹). MOF has pores large enough for lithium ions to permeate through, and its electronically insulating property creates capacitive effects, distributing lithium ions over the surface of the MOF layer to avoid dendrite growth and clogging during lithium plating. Outstanding volumetric and gravimetric capacities (≈940 mAh cm⁻³ and ≈980 mAh g⁻¹) along with exceptional cumulative capacity (≈4.9 Ah cm⁻²) are obtained. This promising approach can store lithium without dendrites to deliver high energy densities required for the current rechargeable batteries.     

Inkjet Printing Flexible Thermoelectric Devices Using Metal Chalcogenide Nanowires

Development of flexible thermoelectric devices offers exciting opportunities for wearable applications in consumer electronics, healthcare, human–machine interface, etc. Despite the increased interests and efforts in nanotechnology-enabled flexible thermoelectrics, translating the superior properties of thermoelectric materials from nanoscale to macroscale and reducing the manufacturing costs at the device level remain a major challenge. Here, an economic and scalable inkjet printing method is reported to fabricate high-performance flexible thermoelectric devices. A general templated-directed chemical transformation process is employed to synthesize several types of 1D metal chalcogenide nanowires (e.g., Ag₂Te, Cu₇Te₄, and Bi₂Te_2.7Se_0.3). These nanowires are made into inks suitable for inkjet printing by dispersing them in ethanol without any additives. As a showcase for thermoelectric applications, fully inkjet-printed Ag₂Te-based flexible films and devices are prepared. The printed films exhibit a power factor of 493.8 µW m⁻¹ K⁻² at 400 K and the printed devices demonstrate a maximum power density of 0.9 µW cm⁻² K⁻², both of which are significantly higher than those reported in state-of-the-art inkjet-printed thermoelectrics. The protocols of metal chalcogenide ink formulations, as well as printing are general and extendable to a wider range of material systems, suggesting the great potential of this printing platform for scalable manufacturing of next-generation, high-performance flexible thermoelectric devices.     

Floating Catalyst Chemical Vapor Deposition Patterning Nitrogen-Doped Single-Walled Carbon Nanotubes for Shape Tailorable and Flexible Micro-Supercapacitors

Micro-supercapacitors (MSCs) as high-power density energy storage units are designed to meet the booming development of flexible electronics, requiring simple and fast fabrication technology. Herein, a fast and direct solvent-free patterning method is reported to fabricate shape-tailorable and flexible MSCs by floating catalyst chemical vapor deposition (FCCVD). The nitrogen-doped single-walled carbon nanotubes (N-SWCNTs) are directly deposited on a patterned filter by FCCVD with designable patterns and facilely dry-transferred on versatile substrates. The obtained MSCs deliver an excellent areal capacitance of 3.6 mF cm⁻² and volumetric capacitance of 98.6 F cm⁻³ at a scan rate of 5 mV s⁻¹ along with excellent long-term cycle stability over 125 000 circles. Furthermore, the MSCs show good performance uniformity, which can be readily integrated via connection in parallel or series to deliver a stable high voltage (4 V with five serially connected devices) and large capacitance (5.1 mF with five parallel devices) at a scan rate of 100 mV s⁻¹, enabling powering the light emitting displays. Therefore, this method blazes the trail of directly preparing flexible, shape-customizable, and high-performance MSCs.     

Wearable Energy Generating and Storing Textile Based on Carbon Nanotube Yarns

The challenges of textiles that can generate and store energy simultaneously for wearable devices are to fabricate yarns that generate electrical energy when stretched, yarns that store this electrical energy, and textile geometries that facilitate these functions. To address these challenges, this research incorporates highly stretchable electrochemical yarn harvesters, where available mechanical strains are large and electrochemical energy storing yarns are achieved by weaving. The solid‐state yarn harvester provides a peak power of 5.3 W kg^?1 for carbon nanotubes. The solid‐state yarn supercapacitor provides stable performance when dynamically deformed by bending and stretching, for example. A textile configuration that consists of harvesters, supercapacitors, and a Schottky diode is produced and stores as much electrical energy as is needed by a serial or parallel connection of the harvesters or supercapacitors. This textile can be applied as a power source for health care devices or other wearable devices and be self‐powered sensors for detecting human motion.     

A Flexible and Safe Planar Zinc-Ion Micro-Battery with Ultrahigh Energy Density Enabled by Interfacial Engineering for Wearable Sensing Systems

Aqueous zinc-ion micro-batteries (ZIMBs) have attracted considerable attention owing to their reliable safety, low cost, and great potential for wearable devices. However, current ZIMBs still suffer from various critical issues, including short cycle life, poor mechanical stability, and inadequate energy density. Herein, the fabrication of flexible planar ZIMBs with ultrahigh energy density by interfacial engineering in the screen-printing process based on high-performance MnO₂-based cathode materials is reported. The Ce-doped MnO₂ (Ce-MnO₂) exhibits significantly enhanced capacity (389.3 mAh g⁻¹), considerable rate capability and admirable cycling stability than that of the pure MnO₂. Importantly, the fabrication of micro-electrodes with ultrahigh mass loading of Ce-MnO₂ (24.12 mg cm⁻²) and good mechanical stability is achieved through optimizing the interfacial bonding between different printed layers. The fabricated planar ZIMBs achieve a record high capacity (7.21 mAh cm⁻² or 497.31 mAh cm⁻³) and energy density (8.43 mWh cm⁻² or 573.45 mWh cm⁻³), as well as excellent flexibility. Besides, a wearable self-powered sensing system for environmental monitoring is further demonstrated by integrating the planar ZIMBs with flexible solar cells and a multifunctional sensor array. This work sheds light on the development of high-performance planar ZIMBs for future self-powered and eco-friendly smart wearable electronics.     

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.     

Liquid‐Gated Transistors Based on Reduced Graphene Oxide for Flexible and Wearable Electronics

Graphene is regarded as the ultimate material for future flexible, high‐performance, and wearable electronics. Herein, a novel, robust, all‐green, highly reliable (yield ≥ 99%), and upscalable technology is reported for wearable applications comprising reduced graphene oxide (rGO) as the electroactive component in liquid‐gated transistors (LGTs). rGO is a formidable material for future flexible and wearable applications due to its easy processability, excellent surface reactivity, and large‐area coverage. A novel protocol is established toward the high‐yield fabrication of flexible rGO LGTs combining high robustness (>1.5 h of continuous operation) with state‐of‐the‐art performances, being similar to those of their rigid counterparts operated under liquid gating, including field‐effect mobility of ≈10^?1 cm² V^?1 s^?1 and transconductance of ≈25 µS. Permeable membranes have been proven crucial to operate flexible LGTs under mechanical stress with reduced amounts of solution (<20 µL). Our rGO LGTs are operated in artificial sweat exploiting two different layouts based on lateral‐flow paper fluidics. These approaches pave the road toward future real‐time tracking of perspiration via a simple and cost‐effective approach. The reported findings contribute to the robust and scalable production of novel graphene‐based flexible devices, whose features fulfill the requirements of wearable electronics.