A New Facile Route to Flexible and Semi‐Transparent Electrodes Based on Water Exfoliated Graphene and their Single‐Electrode Triboelectric Nanogenerator

Wearable technologies are driving current research efforts to self‐powered electronics, for which novel high‐performance materials such as graphene and low‐cost fabrication processes are highly sought.The integration of high‐quality graphene films obtained from scalable water processing approaches in emerging applications for flexible and wearable electronics is demonstrated. A novel method for the assembly of shear exfoliated graphene in water, comprising a direct transfer process assisted by evaporation of isopropyl alcohol is developed. It is shown that graphene films can be easily transferred to any target substrate such as paper, flexible polymeric sheets and fibers, glass, and Si substrates. By combining graphene as the electrode and poly(dimethylsiloxane) as the active layer, a flexible and semi‐transparent triboelectric nanogenerator (TENG) is demonstrated for harvesting energy. The results constitute a new step toward the realization of energy harvesting devices that could be integrated with a wide range of wearable and flexible technologies, and opens new possibilities for the use of TENGs in many applications such as electronic skin and wearable electronics.     

3D Orthogonal Woven Triboelectric Nanogenerator for Effective Biomechanical Energy Harvesting and as Self‐Powered Active Motion Sensors

The development of wearable and large‐area energy‐harvesting textiles has received intensive attention due to their promising applications in next‐generation wearable functional electronics. However, the limited power outputs of conventional textiles have largely hindered their development. Here, in combination with the stainless steel/polyester fiber blended yarn, the polydimethylsiloxane‐coated energy‐harvesting yarn, and nonconductive binding yarn, a high‐power‐output textile triboelectric nanogenerator (TENG) with 3D orthogonal woven structure is developed for effective biomechanical energy harvesting and active motion signal tracking. Based on the advanced 3D structural design, the maximum peak power density of 3D textile can reach 263.36 mW m^?2 under the tapping frequency of 3 Hz, which is several times more than that of conventional 2D textile TENGs. Besides, its collected power is capable of lighting up a warning indicator, sustainably charging a commercial capacitor, and powering a smart watch. The 3D textile TENG can also be used as a self‐powered active motion sensor to constantly monitor the movement signals of human body. Furthermore, a smart dancing blanket is designed to simultaneously convert biomechanical energy and perceive body movement. This work provides a new direction for multifunctional self‐powered textiles with potential applications in wearable electronics, home security, and personalized healthcare.     

Shape Memory Polymers for Body Motion Energy Harvesting and Self‐Powered Mechanosensing

Growing demand in portable electronics raises a requirement to electronic devices being stretchable, deformable, and durable, for which functional polymers are ideal choices of materials. Here, the first transformable smart energy harvester and self‐powered mechanosensation sensor using shape memory polymers is demonstrated. The device is based on the mechanism of a flexible triboelectric nanogenerator using the thermally triggered shape transformation of organic materials for effectively harvesting mechanical energy. This work paves a new direction for functional polymers, especially in the field of mechanosensation for potential applications in areas such as soft robotics, biomedical devices, and wearable electronics.     

Flexible Thermoelectric Materials and Generators: Challenges and Innovations

The urgent need for ecofriendly, stable, long‐lifetime power sources is driving the booming market for miniaturized and integrated electronics, including wearable and medical implantable devices. Flexible thermoelectric materials and devices are receiving increasing attention, due to their capability to convert heat into electricity directly by conformably attaching them onto heat sources. Polymer‐based flexible thermoelectric materials are particularly fascinating because of their intrinsic flexibility, affordability, and low toxicity. There are other promising alternatives including inorganic‐based flexible thermoelectrics that have high energy‐conversion efficiency, large power output, and stability at relatively high temperature. Herein, the state‐of‐the‐art in the development of flexible thermoelectric materials and devices is summarized, including exploring the fundamentals behind the performance of flexible thermoelectric materials and devices by relating materials chemistry and physics to properties. By taking insights from carrier and phonon transport, the limitations of high‐performance flexible thermoelectric materials and the underlying mechanisms associated with each optimization strategy are highlighted. Finally, the remaining challenges in flexible thermoelectric materials are discussed in conclusion, and suggestions and a framework to guide future development are provided, which may pave the way for a bright future for flexible thermoelectric devices in the energy market.     

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.     

Lead‐Free Perovskite Nanowire‐Employed Piezopolymer for Highly Efficient Flexible Nanocomposite Energy Harvester

In the past two decades, mechanical energy harvesting technologies have been developed in various ways to support or power small‐scale electronics. Nevertheless, the strategy for enhancing current and charge performance of flexible piezoelectric energy harvesters using a simple and cost‐effective process is still a challenging issue. Herein, a 1D–3D (1‐3) fully piezoelectric nanocomposite is developed using perovskite BaTiO₃ (BT) nanowire (NW)‐employed poly(vinylidene fluoride‐co‐trifluoroethylene) (P(VDF‐TrFE)) for a high‐performance hybrid nanocomposite generator (hNCG) device. The harvested output of the flexible hNCG reaches up to ≈14 V and ≈4 µA, which is higher than the current levels of even previous piezoceramic film‐based flexible energy harvesters. Finite element analysis method simulations study that the outstanding performance of hNCG devices attributes to not only the piezoelectric synergy of well‐controlled BT NWs and within P(VDF‐TrFE) matrix, but also the effective stress transferability of piezopolymer. As a proof of concept, the flexible hNCG is directly attached to a hand to scavenge energy using a human motion in various biomechanical frequencies for self‐powered wearable patch device applications. This research can pave the way for a new approach to high‐performance wearable and biocompatible self‐sufficient electronics.     

High‐Performance Piezoelectric Nanogenerators with Imprinted P(VDF‐TrFE)/BaTiO3 Nanocomposite Micropillars for Self‐Powered Flexible Sensors

Piezoelectric nanogenerators with large output, high sensitivity, and good flexibility have attracted extensive interest in wearable electronics and personal healthcare. In this paper, the authors propose a high‐performance flexible piezoelectric nanogenerator based on piezoelectrically enhanced nanocomposite micropillar array of polyvinylidene fluoride‐trifluoroethylene (P(VDF‐TrFE))/barium titanate (BaTiO₃) for energy harvesting and highly sensitive self‐powered sensing. By a reliable and scalable nanoimprinting process, the piezoelectrically enhanced vertically aligned P(VDF‐TrFE)/BaTiO₃ nanocomposite micropillar arrays are fabricated. The piezoelectric device exhibits enhanced voltage of 13.2 V and a current density of 0.33 µA cm^?2, which an enhancement by a factor of 7.3 relatives to the pristine P(VDF‐TrFE) bulk film. The mechanisms of high performance are mainly attributed to the enhanced piezoelectricity of the P(VDF‐TrFE)/BaTiO₃ nanocomposite materials and the improved mechanical flexibility of the micropillar array. Under mechanical impact, stable electricity is stably generated from the nanogenerator and used to drive various electronic devices to work continuously, implying its significance in the field of consumer electronic devices. Furthermore, it can be applied as self‐powered flexible sensor work in a noncontact mode for detecting air pressure and wearable sensors for detecting some human vital signs including different modes of breath and heartbeat pulse, which shows its potential applications in flexible electronics and medical sciences.     

On‐Skin Triboelectric Nanogenerator and Self‐Powered Sensor with Ultrathin Thickness and High Stretchability

Researchers have devoted a lot of efforts on pursuing light weight and high flexibility for the wearable electronics, which also requires the related energy harvesting devices to have ultrathin thickness and high stretchability. Hence, an elastic triboelectric nanogenerator (TENG) is proposed that can serve as the second skin on human body. The total thickness of this TENG is about 102 µm and the device can work durably under a strain of 100%. The carbon grease is painted on the surface of elastomer film to work as stretchable electrode and thus the fine geometry control of the electrode can be achieved. This elastic TENG can even work on the human fingers without disturbing body movement. The open‐circuit voltage and short‐circuit current from the device with a contact area of 9 cm² can reach 115 V and 3 µA, respectively. Two kinds of self‐powered sensor systems with optimized identification strategies are also designed to demonstrate the application possibility of this elastic TENG. The superior characteristics of ultrathin thickness, high stretchability, and fine geometry control of this TENG can promote many potential applications in the field of wearable self‐powered sensory system, electronics skin, artificial muscles, and soft robotics.     

柔性热电发电器的关键工艺及其展望

热电发电器是固态能量收集器,以可靠和可再生的方式将热能转换成电能。过去几年的研究表明,人体的热量可以很好地被柔性热电发电器转换为电能并加以利用。与用于可穿戴设备的其他传统发电器相比,柔性热电发电器可利用低品位的热能发电且环境友好。柔性热电发电器将有可能为任何无线传感器节点提供足够的能量(通常功率要求小于毫瓦级)。本文综述了热电发电器的概况,重点介绍了制造柔性热电发电器的关键工艺,讨论了热电发电器的基本原理、效率、应用以及存在的一些问题。     

Service Behavior of Multifunctional Triboelectric Nanogenerators

Triboelectric nanogenerators (TENGs) or TENG‐based self‐charging systems harvesting energy from ambient environment are promising power solution for electronics. The stable running remains a key consideration in view of potential complex application environment. In this work, a textile‐based tailorable multifunctional TENG (T‐TENG) is developed. The T‐TENG is used as self‐powered human body motion sensor, water energy harvester, and formed all textile‐based flexible self‐charging system by integrating with textile‐based supercapacitors. The service behavior and the mechanism of performance retention are also studied when the T‐TENG is damaged. As a self‐powered human body motion sensor, the T‐TENG maintains the stable properties when it is cut. As a water energy harvester, the T‐TENG is capable of scavenging mechanical energy from water efficiently even if it is damaged partly. Besides, the charge properties of the self‐charging system are systematically investigated when the T‐TENG is cut. The investigation on service behavior of T‐TENG and TENG‐based self‐charging system pushes forward the development of highly reliable electronics and is a guide for other nanodevices and nanosystems.     

Thermoelectric textile devices with thin films of nanocellulose and copper iodide

Owing to the rapid development of wearable electronics and smart textiles, demands for flexible and wearable thermoelectric (TE) devices, which can generate electricity in a ubiquitous, unintermittent and noiseless way for on-body applications are growing rapidly. Due to the inherent flexibility and wearability features, textile-based thermoelectric generators (TEGs) possess significant potential for biomedical and consumer health and safety applications. In this study, using commercial cotton fabric, we created efficient thermoelectric (TE) textile that, unlike analogs, is based on thin-film composite of biocompatible semiconductor copper iodide (CuI) and biodegradable polymer nanocellulose (NC_p) obtained by processing a widespread plant common reed. The CuI films with average thickness 10 µm were deposited via low-temperature aqueous cheap, facile, and scalable fabrication technique Successive Ionic Layer Adsorption and Reaction (SILAR). The NC_p sublayer made it possible to fabricate thin-film ohmic contacts through vacuum deposition of chromium on the nanostructured CuI film in the TE textile. The topping of CuI film with NC_p layer improved durability and wear resistance of the wearable thermoelectric module fabricated with this TE textile. The developed TE module has shown output power density 44 µW/cm² at temperature gradient 50 K that is among the best currently known results for solid miniature flexible and fabric-based TEGs.

     

Fiber/Fabric-Based Piezoelectric and Triboelectric Nanogenerators for Flexible/Stretchable and Wearable Electronics and Artificial Intelligence

Integration of advanced nanogenerator technology with conventional textile processes fosters the emergence of textile-based nanogenerators (NGs), which will inevitably promote the rapid development and widespread applications of next-generation wearable electronics and multifaceted artificial intelligence systems. NGs endow smart textiles with mechanical energy harvesting and multifunctional self-powered sensing capabilities, while textiles provide a versatile flexible design carrier and extensive wearable application platform for their development. However, due to the lack of an effective interactive platform and communication channel between researchers specializing in NGs and those good at textiles, it is rather difficult to achieve fiber/fabric-based NGs with both excellent electrical output properties and outstanding textile-related performances. To this end, a critical review is presented on the current state of the arts of wearable fiber/fabric-based piezoelectric nanogenerators and triboelectric nanogenerators with respect to basic classifications, material selections, fabrication techniques, structural designs, and working principles, as well as potential applications. Furthermore, the potential difficulties and tough challenges that can impede their large-scale commercial applications are summarized and discussed. It is hoped that this review will not only deepen the ties between smart textiles and wearable NGs, but also push forward further research and applications of future wearable fiber/fabric-based NGs.     

Advanced Carbon for Flexible and Wearable Electronics

Flexible and wearable electronics are attracting wide attention due to their potential applications in wearable human health monitoring and care systems. Carbon materials have combined superiorities such as good electrical conductivity, intrinsic and structural flexibility, light weight, high chemical and thermal stability, ease of chemical functionalization, as well as potential mass production, enabling them to be promising candidate materials for flexible and wearable electronics. Consequently, great efforts are devoted to the controlled fabrication of carbon materials with rationally designed structures for applications in next‐generation electronics. Herein, the latest advances in the rational design and controlled fabrication of carbon materials toward applications in flexible and wearable electronics are reviewed. Various carbon materials (carbon nanotubes, graphene, natural‐biomaterial‐derived carbon, etc.) with controlled micro/nanostructures and designed macroscopic morphologies for high‐performance flexible electronics are introduced. The fabrication strategies, working mechanism, performance, and applications of carbon‐based flexible devices are reviewed and discussed, including strain/pressure sensors, temperature/humidity sensors, electrochemical sensors, flexible conductive electrodes/wires, and flexible power devices. Furthermore, the integration of multiple devices toward multifunctional wearable systems is briefly reviewed. Finally, the existing challenges and future opportunities in this field are summarized.     

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.     

A Shape‐Adaptive Thin‐Film‐Based Approach for 50% High‐Efficiency Energy Generation Through Micro‐Grating Sliding Electrification

Effectively harvesting ambient mechanical energy is the key for realizing self‐powered and autonomous electronics, which addresses limitations of batteries and thus has tremendous applications in sensor networks, wireless devices, and wearable/implantable electronics, etc. Here, a thin‐film‐based micro‐grating triboelectric nanogenerator (MG‐TENG) is developed for high‐efficiency power generation through conversion of mechanical energy. The shape‐adaptive MG‐TENG relies on sliding electrification between complementary micro‐sized arrays of linear grating, which offers a unique and straightforward solution in harnessing energy from relative sliding motion between surfaces. Operating at a sliding velocity of 10 m/s, a MG‐TENG of 60 cm² in overall area, 0.2 cm³ in volume and 0.6 g in weight can deliver an average output power of 3 W (power density of 50 mW cm^?2 and 15 W cm^?3) at an overall conversion efficiency of ～50%, making it a sufficient power supply to regular electronics, such as light bulbs. The scalable and cost‐effective MG‐TENG is practically applicable in not only harvesting various mechanical motions but also possibly power generation at a large scale.     

Hybrid Energy Harvesters: Toward Sustainable Energy Harvesting

Recently, sustainable green energy harvesting systems have been receiving great attention for their potential use in self‐powered smart wireless sensor network (WSN) systems. In particular, though the developed WSN systems are able to advance public good, very high and long‐term budgets will be required in order to use them to supply electrical energy through temporary batteries or connecting power cables. This report summarizes recent significant progress in the development of hybrid nanogenerators for a sustainable energy harvesting system that use natural and artificial energies such as solar, wind, wave, heat, machine vibration, and automobile noise. It starts with a brief introduction of energy harvesting systems, and then summarizes the different hybrid energy harvesting systems: integration of mechanical and photovoltaic energy harvesters, integration of mechanical and thermal energy harvesters, integration of thermal and photovoltaic energy harvesters, and others. In terms of the reported hybrid nanogenerators, a systematic summary of their structures, working mechanisms, and output performances is provided. Specifically, electromagnetic induction, triboelectric, piezoelectric, photovoltaic, thermoelectric, and pyroelectric effects are reviewed on the basis of the individual and hybrid power performances of hybrid nanogenerators and their practical applications with various device designs. Finally, the perspectives on and challenges in developing high performance and sustainable hybrid nanogenerator systems are presented.     

聚3, 4-乙烯二氧噻吩: 聚苯乙烯磺酸盐基柔性复合热电材料研究进展

热电材料可以实现热能与电能的直接转化,是一种安全环保的新型能源材料。近年来,随着可穿戴电子设备的发展,柔性热电材料成为研究人员关注的焦点。传统无机热电材料具有优异的热电性能,但由于自身固有的脆性,限制了在柔性领域的发展。聚3, 4-乙烯二氧噻吩: 聚苯乙烯磺酸盐(PEDOT: PSS)具有高电导率、低热导率和良好的柔性,在柔性热电领域具有巨大的潜力。当选择合适的无机填料与PEDOT: PSS进行复合,可以得到优异的热电性能和良好的力学性能。本文综述了PEDOT: PSS基纳米复合薄膜的最新进展,并详细介绍了提高PEDOT: PSS基纳米复合薄膜热电性能的有效方法。最后,本文总结了实现高性能PEDOT: PSS基柔性热电材料的途径及面对的挑战。      

Materials and Designs for Wearable Photodetectors

Photodetectors (PDs), as an indispensable component in electronics, are highly desired to be flexible to meet the trend of next‐generation wearable electronics. Unfortunately, no in‐depth reviews on the design strategies, material exploration, and potential applications of wearable photodetectors are found in literature to date. Thus, this progress report first summarizes the fundamental design principles of turning “hard” photodetectors “soft,” including 2D (polymer and paper substrate‐based devices) and 1D PDs (fiber shaped devices). In short, the flexibility of PDs is realized through elaborate substrate modification, material selection, and device layout. More importantly, this report presents the current progress and specific requirements for wearable PDs according to the application: monitoring, imaging, and optical communication. Challenges and future research directions in these fields are proposed at the end. The purpose of this progress report is not only to shed light on the basic design principles of wearable PDs, but also serve as the roadmap for future exploration in wearable PDs in various applications, including health monitoring and Internet of Things.     

Cellulose‐Based Nanomaterials for Energy Applications

Cellulose is the most abundant natural polymer on earth, providing a sustainable green resource that is renewable, degradable, biocompatible, and cost effective. Recently, nanocellulose‐based mesoporous structures, flexible thin films, fibers, and networks are increasingly developed and used in photovoltaic devices, energy storage systems, mechanical energy harvesters, and catalysts components, showing tremendous materials science value and application potential in many energy‐related fields. In this Review, the most recent advancements of processing, integration, and application of cellulose nanomaterials in the areas of solar energy harvesting, energy storage, and mechanical energy harvesting are reviewed. For solar energy harvesting, promising applications of cellulose‐based nanostructures for both solar cells and photoelectrochemical electrodes development are reviewed, and their morphology‐related merits are discussed. For energy storage, the discussion is primarily focused on the applications of cellulose‐based nanomaterials in lithium‐ion batteries, including electrodes (e.g., active materials, binders, and structural support), electrolytes, and separators. Applications of cellulose nanomaterials in supercapacitors are also reviewed briefly. For mechanical energy harvesting, the most recent technology evolution in cellulose‐based triboelectric nanogenerators is reviewed, from fundamental property tuning to practical implementations. At last, the future research potential and opportunities of cellulose nanomaterials as a new energy material are discussed.     

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.