Self‐Healing,Flexible, and Tailorable Triboelectric Nanogenerators for Self‐Powered Sensors based on Thermal Effect of Infrared Radiation

Self‐healing triboelectric nanogenerators (TENGs) with flexibility, robustness, and conformability are highly desirable for promising flexible and wearable devices, which can serve as a durable, stable, and renewable power supply, as well as a self‐powered sensor. Herein, an entirely self‐healing, flexible, and tailorable TENG is designed as a wearable sensor to monitor human motion, with infrared radiation from skin to promote self‐healing after being broken based on thermal effect of infrared radiation. Human skin is a natural infrared radiation emitter, providing favorable conditions for the device to function efficiently. The reversible imine bonds and quadruple hydrogen bonding (UPy) moieties are introduced into polymer networks to construct self‐healable electrification layer. UPy‐functionalized multiwalled carbon nanotubes are further incorporated into healable polymer to obtain conductive nanocomposite. Driven by the dynamic bonds, the designed and synthesized materials show excellent intrinsic self‐healing and shape‐tailorable features. Moreover, there is a robust interface bonding in the TENG devices due to the similar healable networks between electrification layer and electrode. The output electric performances of the self‐healable TENG devices can almost restore their original state when the damage of the devices occurs. This work presents a novel strategy for flexible devices, contributing to future sustainable energy and wearable electronics.     

Recent Progress of Flexible Photodetectors Based on Low-Dimensional II–VI Semiconductors and Their Application in Wearable Electronics

Flexible photodetectors exhibit many advantages such as a good bendability, foldability, and even stretchability as well as weight light, which have triggered a widely concerned in wearable electronics including wearable monitoring, wearable image sensing, self-powered integrated electronics, etc. Recently, various II–VI semiconductor nanostructures have become promising candidates in flexible photodetectors due to their unique characteristics, such as direct bandgap semiconductors, excellent optical and electric properties, high quantum efficiency, and inherent mechanical flexibility. Herein, the most recent progress on low-dimensional (0D, 1D, 2D, and related heterostructures) II–VI semiconductors based flexible photodetectors and their application in wearable electronic is reviewed. First, a brief introduction of the main sensing mechanisms and key figures of merits for photodetectors is presented. Then, the recent progresses on flexible photodetectors are provided, in which the functional materials synthesis methods are also discussed. More importantly, the applications of the flexible photodetectors are summarized, including wearable monitoring sensors, image sensors, and self-powered integrated wearable electronics. Finally, the challenges and the future research direction of the flexible photodetectors are discussed, meanwhile the outlook for the development of flexible photodetectors in the future integration of wearable electronic is also provided.     

Recent advances in flexible and wearable organic optoelectronic devices

Flexible and wearable optoelectronic devices have been developing to a new stage due to their unique capacity for the possibility of a variety of wearable intelligent electronics,including bendable smartphones,foldable touch screens and antennas,paper-like displays,and curved and flexible solid-state lighting devices.Before extensive commercial applications,some issues still have to be solved for flexible and wearable optoelectronic devices.In this regard,this review concludes the newly emerging flexible substrate materials,transparent conductive electrodes,device architectures and light manipulation methods.Examples of these components applied for various kinds of devices are also summarized.Finally,perspectives about the bright future of flexible and wearable electronic devices are proposed.     

Wearable Force Touch Sensor Array Using a Flexible and Transparent Electrode

Transparent electrodes have been widely used for various electronics and optoelectronics, including flexible ones. Many nanomaterial‐based electrodes, in particular 1D and 2D nanomaterials, have been proposed as next‐generation transparent and flexible electrodes. However, their transparency, conductivity, large‐area uniformity, and sometimes cost are not yet sufficient to replace indium tin oxide (ITO). Furthermore, the conventional ITO is quite rigid and susceptible to mechanical fractures under deformations (e.g., bending, folding). In this study, the authors report new advances in the design, fabrication, and integration of wearable and transparent force touch (touch and pressure) sensors by exploiting the previous efforts in stretchable electronics as well as novel ideas in the transparent and flexible electrode. The optical and mechanical experiment, along with simulation results, exhibit the excellent transparency, conductivity, uniformity, and flexibility of the proposed epoxy‐copper‐ITO (ECI) multilayer electrode. By using this multi‐layered ECI electrode, the authors present a wearable and transparent force touch sensor array, which is multiplexed by Si nanomembrane p‐i‐n junction‐type (PIN) diodes and integrated on the skin‐mounted quantum dot light‐emitting diodes. This novel integrated system is successfully applied as a wearable human–machine interface (HMI) to control a drone wirelessly. These advances in novel material structures and system‐level integration strategies create new opportunities in wearable smart displays.     

A High‐Capacitance Salt‐Free Dielectric for Self‐Healable,Printable, and Flexible Organic Field Effect Transistors and Chemical Sensor

Printable and flexible electronics attract sustained attention for their low cost, easy scale up, and potential application in wearable and implantable sensors. However, they are susceptible to scratching, rupture, or other damage from bending or stretching due to their “soft” nature compared to their rigid counterparts (Si‐based electronics), leading to loss of functionality. Self‐healing capability is highly desirable for these “soft” electronic devices. Here, a versatile self‐healing polymer blend dielectric is developed with no added salts and it is integrated into organic field transistors (OFETs) as a gate insulator material. This polymer blend exhibits an unusually high thin film capacitance (1400 nF cm^?2 at 120 nm thickness and 20–100 Hz). Furthermore, it shows pronounced electrical and mechanical self‐healing behavior, can serve as the gate dielectric for organic semiconductors, and can even induce healing of the conductivity of a layer coated above it together with the process of healing itself. Based on these attractive properties, we developed a self‐healable, low‐voltage operable, printed, and flexible OFET for the first time, showing promise for vapor sensing as well as conventional OFET applications.     

Graphene-based flexible and wearable electronics

Graphene with an exceptional combination of electronic,optical and outstanding mechanical features has been proved to lead a completely different kind of 2-D electronics.The most exciting feature of graphene is its ultra-thin thickness,that can be conformally contacted to any kind of rough surface without losing much of its transparency and conductivity.Graphene has been explored demonstrating various prototype flexible electronic applications,however,its potentiality has been proven wherever transparent conductive electrodes (TCEs) are needed in a flexible,stretchable format.Graphene-based TCEs in flexible electronic applications showed greatly superior performance over their conventionally available competitor indium tin oxide (ITO).Moreover,enormous applications have been emerging,especially in wearable devices that can be potentially used in our daily life as well as in biomedical areas.However,the production of high-quality,defect-free large area graphene is still a challenge and the main hurdle in the commercialization of flexible and wearable products.The objective of the present review paper is to summarize the progress made so far in graphene-based flexible and wearable applications.The current developments including challenges and future perspectives are also highlighted.     

Thermally Controlled,Patterned Graphene Transfer Printing for Transparent and Wearable Electronic/Optoelectronic System

Graphene has been highlighted as a platform material in transparent electronics and optoelectronics, including flexible and stretchable ones, due to its unique properties such as optical transparency, mechanical softness, ultrathin thickness, and high carrier mobility. Despite huge research efforts for graphene‐based electronic/optoelectronic devices, there are remaining challenges in terms of their seamless integration, such as the high‐quality contact formation, precise alignment of micrometer‐scale patterns, and control of interfacial‐adhesion/local‐resistance. Here, a thermally controlled transfer printing technique that allows multiple patterned‐graphene transfers at desired locations is presented. Using the thermal‐expansion mismatch between the viscoelastic sacrificial layer and the elastic stamp, a “heating and cooling” process precisely positions patterned graphene layers on various substrates, including graphene prepatterns, hydrophilic surfaces, and superhydrophobic surfaces, with high transfer yields. A detailed theoretical analysis of underlying physics/mechanics of this approach is also described. The proposed transfer printing successfully integrates graphene‐based stretchable sensors, actuators, light‐emitting diodes, and other electronics in one platform, paving the way toward transparent and wearable multifunctional electronic systems.     

Flexible Transparent Reduced Graphene Oxide Sensor Coupled with Organic Dye Molecules for Rapid Dual‐Mode Ammonia Gas Detection

Flexible chemical sensors utilizing chemically sensitive nanomaterials are of great interest for wearable sensing applications. However, obtaining high performance flexible chemical sensors with high sensitivity, fast response, transparency, stability, and workability at ambient conditions is still challenging. Herein, a newly designed flexible and transparent chemical sensor of reduced graphene oxide (R‐GO) coupled with organic dye molecules (bromophenol blue) is introduced. This device has promising properties such as high mechanical flexibility (>5000 bending cycles with a bending radius of 0.95 cm) and optical transparency (>60% in the visible region). Furthermore, stacking the water‐trapping dye layer on R‐GO enables a higher response as well as workability in a large relative humidity range (up to 80%), and dual‐mode detection capabilities of colorimetric and electrical sensing for NH₃ gas (5–40 ppm). These advantageous attributes of the flexible and transparent R‐GO sensor coupled with organic dye molecules provide great potential for real‐time monitoring of toxic gas/vapor in future practical chemical sensing at room conditions in wearable electronics.     

Quasifractal Networks as Current Collectors for Transparent Flexible Supercapacitors

A high performance, transparent, and simultaneously mechanically flexible supercapacitor, with electrodes based on a bio‐inspired, quasifractal metallic network is demonstrated. Excellent performance parameters, such as the specific capacitance of 5.6 mF cm^?2 (at 45% transparency), great long‐term electrochemical and mechanical stability under stress, and low cost, make this one of the best reported, and most promising candidates for applications in the wearable, transparent integrated electronics.     

Highly Stretchable or Transparent Conductor Fabrication by a Hierarchical Multiscale Hybrid Nanocomposite

As is frequently seen in sci‐fi movies, future electronics are expected to ultimately be in the form of wearable electronics. To realize wearable electronics, the electric components should be soft, flexible, and even stretchable to be human‐friendly. An important step is presented toward realization of wearable electronics by developing a hierarchical multiscale hybrid nanocomposite for highly flexible, stretchable, or transparent conductors. The hybrid nanocomposite combines the enhanced mechanical compliance, electrical conductivity, and optical transparency of small CNTs (d ≈ 1.2 nm) and the enhanced electrical conductivity of relatively bigger Ag nanowire (d ≈ 150 nm) backbone to provide efficient multiscale electron transport path with Ag nanowire current backbone collector and local CNT percolation network. The highly elastic hybrid nanocomposite conductors and highly transparent flexible conductors can be mounted on any non‐planar or soft surfaces to realize human‐friendly electronics interface for future wearable electronics.     

Integrating Flexible Ultralight 3D Ni Micromesh Current Collector with NiCo Bimetallic Hydroxide for Smart Hybrid Supercapacitors

Flexible and lightweight supercapacitors with superior mechanical flexibility and outstanding capacity are regarded as an ideal power source for wearable electronic devices. Meanwhile, incorporating additional novel characters such as transparency and electrochromism can further benefit the development of smart supercapacitors. Nevertheless, the application of the commonly used planar-structural current collectors is seriously restricted by their intrinsic properties such as poor rigidity, large thickness, and limited loading surface area. Flexible and ultralight current collectors with 3D architecture, high conductivity, and easy integration are believed to be the most appropriate alternatives to build high-performance supercapacitors. In this study, a novel and scalable manufacturing technique is developed to produce a flexible and ultralight 3D Ni micromesh (3D NM) current collector for supercapacitor. Flexible smart supercapacitor integrated by 3D NM and high active Ni–Co bimetallic hydroxide (3D NM@NiCo BH) delivers a considerable rate performance (60.6% capacity retention from 1 to 50 mA cm⁻²). Furthermore, the fabricated hybrid supercapacitor device integrated with electrochromic functionality can visually indicate the energy level by a color display. This flexible electrochromic supercapacitor based on ultralight 3D Ni micromesh provides a novel insight into multifunctional energy storage systems for smart wearable electronic devices.     

Flexible Breathable Nanomesh Electronic Devices for On‐Demand Therapy

Flexible electronics are drawing tremendous interest for various applications in wearable healthcare biomonitoring, on‐demand therapy, and human–machine interactions. However, conventional plastic substrates with uncomfortableness, mechanical mismatches, and impermeability have limited the application of flexible on‐skin electronic devices for healthcare biomonitoring and on‐demand therapy. Herein, flexible breathable electronic devices with the capabilities of real‐time temperature sensing and timely on‐demand anti‐infection therapy at wound sites are presented. These devices are assembled from a crosslinked electrospun moxifloxacin hydrochloride (MOX)‐loaded thermoresponsive polymer nanomesh film with a conductive pattern. The conductive polymer nanomesh film demonstrates excellent flexibility, reliable breathability, and robust environmental stability. Furthermore, the assembled temperature sensor displays a linear relationship between the electrical resistance and temperature, potentially enabling real‐time biomonitoring of tissue temperature at the wound site. Smart artificial electronic skins (E‐skins) are assembled from the thermoresponsive polymer nanomesh film for spatial touching sensing mapping of temperature changes. Furthermore, the flexible temperature sensor is coupled with a wireless transmitter for real‐time wireless temperature monitoring. Notably, the thermoresponsive polymer nanomesh film can also be assembled as a highly efficient flexible heater to trigger the on‐demand release of antibiotics loaded in the fibers to eliminate bacterial colonization in the wound site once infection has occurred.     

Flexible Transparent Supercapacitors: Materials and Devices

The progressive development of flexible transparent portable electronic devices is in urgent need of matching power sources. Flexible transparent supercapacitors (FTSCs) are the core resources due to their high optical transmittance, endurable mechanical flexibility, excellent electrochemical performance, and facilely accessible device configuration. This review organizes the rational design of nanostructured electrode materials toward FTSCs. First, the structure, mechanism, and property of FTSCs are introduced. Then, the design principles of diverse electrode materials are discussed to achieve flexible transparent conductive electrodes (FTCEs) with different figure of merits (both electrical FoMe and capacitive FoMc), mechanical strength, and environmental stability. Following the achievements in multifunctional FTSCs focusing on film-supercapacitors, micro-supercapacitors, electrochromic supercapacitors, photo-supercapacitors, and battery-like supercapacitors are also highlighted. Finally, the current challenges and future perspectives on viable materials in the construction of FTSCs to power portable electronics are outlined.     

Flexible and Transparent Graphene Electrode Architecture with Selective Defect Decoration for Organic Light‐Emitting Diodes

Graphene produced by chemical vapor deposition (CVD) has attracted great interest as a transparent conducting material, due to its extraordinary characteristics such as flexibility, optical transparency, and high conductivity, especially in next‐generation displays. Graphene‐based novel electrodes have the potential to satisfy the important factors for high‐performance flexible organic light‐emitting diodes (OLEDs) in terms of sheet resistance, transmittance, work function, and surface roughness. In this study, flexible and transparent graphene electrode architecture is proposed by adopting a selective defect healing technique for CVD‐grown graphene, which results in several benefits that produce high‐performance devices with excellent stabilities. The proposed architecture, which has a multi‐layer graphene structure treated by a layer‐by‐layer healing process, exhibits significant improvement in sheet resistance with high optical transparency. For improving the charge transport property and mechanical robustness, various defect sites of the CVD‐grown graphene are successfully decorated with gold nanoparticles through a simple electroplating (EP) method. Further, a graphene‐based OLED device that integrates the proposed electrode architecture on flexible substrates is demonstrated. Therefore, this architecture provides a new strategy to fabricate graphene electrode in OLEDs, extending graphene's immense potential as an advanced conductor toward high‐performance, flexible, and transparent displays.     

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

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

Screen‐Printed Poly(3,4‐Ethylenedioxythiophene):Poly(Styrenesulfonate) Grids as ITO‐Free Anodes for Flexible Organic Light‐Emitting Diodes

Poly(3,4‐ethylenedioxythiophene):poly(styrenesulfonate) (PEDOT: PSS) grids have been successfully constructed by roll‐to‐roll compatible screen‐printing techniques and have been used as indium tin oxide (ITO)‐free anodes for flexible organic light‐emitting diodes (OLEDs). The grid‐type transparent conductive electrodes (TCEs) can adopt thicker PEDOT: PSS grid lines to ensure the conductivity, while the mesh‐like grid structure can play an important role to maintain high optical transparency. By adjusting grid periods, grid thickness and treatment of organic additives, PEDOT: PSS TCEs with high optical transparency, low sheet resistance, and excellent mechanical flexibility have been achieved. Using the screen‐printed PEDOT: PSS grids as the anodes, ITO‐free OLEDs achieved peak current efficiency of 3.40 cd A^?1 at the current density of 10 mA cm^?2, which are 1.56 times better than the devices with ITO glass as the anodes. The improved efficiency is attributed to the light extraction effect and improved transparency by the grid structure. The superior optoelectronic performances of OLEDs based on flexible screen‐printed PEDOT: PSS grid anodes suggest their great prospects as ITO‐free anodes for flexible and wearable electronic applications.     

Entirely,Intrinsically, and Autonomously Self‐Healable,Highly Transparent,and Superstretchable Triboelectric Nanogenerator for Personal Power Sources and Self‐Powered Electronic Skins

Power and electronic components that are self‐healable, deformable, transparent, and self‐powered are highly desirable for next‐generation energy/electronic/robotic applications. Here, an energy‐harvesting triboelectric nanogenerator (TENG) that combines the above features is demonstrated, which can serve not only as a power source but also as self‐powered electronic skin. This is the first time that both of the triboelectric‐charged layer and electrode of the TENG are intrinsically and autonomously self‐healable at ambient conditions. Additionally, comparing with previous partially healable TENGs, its fast healing time (30 min, 100% efficiency at 900% strain), high transparency (88.6%), and inherent superstretchability (>900%) are much more favorable. It consists of a metal‐coordinated polymer as the triboelectrically charged layer and hydrogen‐bonded ionic gel as the electrode. Even after 500 cutting‐and‐healing cycles or under extreme 900%‐strain, the TENG retains its functionality. The generated electricity can be used directly or stored to power commercial electronics. The TENG is further used as self‐powered tactile‐sensing skin in diverse human–machine interfaces including smart glass, an epidermal controller, and phone panel. This TENG with merits including fast ambient‐condition self‐healing, high transparency, intrinsic stretchability, and energy‐extraction and actively‐sensing abilities, can meet wide application needs ranging from deformable/portable/transparent electronics, smart interfaces, to artificial skins.     

Hybrid Smart Fiber with Spontaneous Self‐Charging Mechanism for Sustainable Wearable Electronics

Smart wearable electronics that are fabricated on light‐weight fabrics or flexible substrates are considered to be of next‐generation and portable electronic device systems. Ideal wearable and portable applications not only require the device to be integrated into various fiber form factors, but also desire self‐powered system in such a way that the devices can be continuously supplied with power as well as simultaneously save the acquired energy for their portability and sustainability. Nevertheless, most of all self‐powered wearable electronics requiring both the generation of the electricity and storing of the harvested energy, which have been developed so far, have employed externally connected individual energy generation and storage fiber devices using external circuits. In this work, for the first time, a hybrid smart fiber that exhibits a spontaneous energy generation and storage process within a single fiber device that does not need any external electric circuit/connection is introduced. This is achieved through the employment of asymmetry coaxial structure in an electrolyte system of the supercapacitor that creates potential difference upon the creation of the triboelectric charges. This development in the self‐charging technology provides great opportunities to establish a new device platform in fiber/textile‐based electronics.     

Polyelectrolyte Dielectrics for Flexible Low‐Voltage Organic Thin‐Film Transistors in Highly Sensitive Pressure Sensing

Organic thin‐film transistors (OTFTs) can provide an effective platform to develop flexible pressure sensors in wearable electronics due to their good signal amplification function. However, it is particularly difficult to realize OTFT‐based pressure sensors with both low‐voltage operation and high sensitivity. Here, controllable polyelectrolyte composites based on poly(ethylene glycol) (PEG) and polyacrylic acid (PAA) are developed as a type of high‐capacitance dielectrics for flexible OTFTs and ultrasensitive pressure sensors with sub‐1 V operation. Flexible OTFTs using the PAA:PEG dielectrics show good universality and greatly enhanced electrical performance under a much smaller operating voltage of ?0.7 V than those with a pristine PAA dielectric. The low‐voltage OTFTs also exhibit excellent flexibility and bending stability under various bending radii and long cycles. Flexible OTFT‐based pressure sensors with low‐voltage operation and superhigh sensitivity are demonstrated by using a suspended semiconductor/dielectric/gate structure in combination with the PAA:PEG dielectric. The sensors deliver a record high sensitivity of 452.7 kPa^?1 under a low‐voltage of ?0.7 V, and excellent operating stability over 5000 cycles. The OTFT sensors can be built into a wearable sensor array for spatial pressure mapping, which shows a bright potential in flexible electronics such as wearable devices and smart skins.     

Recent Progress in Flexible and Stretchable Organic Solar Cells

Flexible and stretchable organic solar cells (OSCs) have attracted enormous attention due to their potential applications in wearable and portable devices. To achieve flexibility and stretchability, many efforts have been made with regard to mechanically robust electrodes, interface layers, and photoactive semiconductors. This has greatly improved the performance of the devices. State‐of‐the‐art flexible and stretchable OSCs have achieved a power conversion efficiency of 15.21% (16.55% for tandem flexible devices) and 13%, respectively. Here, the recent progress of flexible and stretchable OSCs in terms of their components and processing methods are summarized and discussed. The future challenges and perspectives for flexible and stretchable OSCs are also presented.