A Flexible Stretchable Hydrogel Electrolyte for Healable All‐in‐One Configured Supercapacitors

The development of integrated high‐performance supercapacitors with all‐in‐one configuration, excellent flexibility and autonomously intrinsic self‐healability, and without the extra healable film layers, is still tremendously challenging. Compared to the sandwich‐like laminated structures of supercapacitors with augmented interfacial contact resistance, the flexible healable integrated supercapacitor with all‐in‐one structure could theoretically improve their interfacial contact resistance and energy densities, simplify the tedious device assembly process, prolong the lifetime, and avoid the displacement and delamination of multilayered configurations under deformations. Herein, a flexible healable all‐in‐one configured supercapacitor with excellent flexibility and reliable self‐healing ability by avoiding the extra healable film substrates and the postassembled sandwich‐like laminated structures is developed. The healable all‐in‐one configured supercapacitor is prepared from in situ polymerization and deposition of nanocomposites electrode materials onto the two‐sided faces of the self‐healing hydrogel electrolyte separator. The self‐healing hydrogel film is obtained from the physically crosslinked hydrogel with enormous hydrogen bonds, which can endow the healable capability through dynamic hydrogen bonding. The assembled all‐in‐one configured supercapacitor exhibits enhanced capacitive performance, good cycling stability, reliable self‐healing capability, and excellent flexibility. It holds broad prospects for obtaining various flexible healable all‐in‐one configured supercapacitors for working as portable energy storage devices in wearable electronics.     

Flexible Transparent Films Based on Nanocomposite Networks of Polyaniline and Carbon Nanotubes for High‐Performance Gas Sensing

A flexible, transparent, chemical gas sensor is assembled from a transparent conducting film of carbon nanotube (CNT) networks that are coated with hierarchically nanostructured polyaniline (PANI) nanorods. The nanocomposite film is synthesized by in‐situ, chemical oxidative polymerization of aniline in a functional multiwalled CNT (FMWCNT) suspension and is simultaneously deposited onto a flexible polyethylene terephthalate (PET) substrate. An as‐prepared flexible transparent chemical gas sensor exhibits excellent transparency of 85.0% at 550 nm using the PANI/FMWCNT nanocomposite film prepared over a reaction time of 8 h. The sensor also shows good flexibility, without any obvious decrease in performance after 500 bending/extending cycles, demonstrating high‐performance, portable gas sensing at room temperature. This superior performance could be attributed to the improved electron transport and collection due to the CNTs, resulting in reliable and efficient sensing, as well as the high surface‐to‐volume ratio of the hierarchically nanostructured composites. The excellent transparency, improved sensing performance, and superior flexibility of the device, may enable the integration of this simple, low‐cost, gas sensor into handheld flexible transparent electronic circuitry and optoelectronic devices.     

A Highly Stretchable and Real‐Time Healable Supercapacitor

In addition to a high specific capacitance, a large stretchability and self‐healing properties are also essential to improve the practicality and reliability of supercapacitors in portable and wearable electronics. However, the integration of multiple functions into one device remains challenging. Here, the construction of a highly stretchable and real‐time omni‐healable supercapacitor is demonstrated by sandwiching the polypyrrole‐incorporated gold nanoparticle/carbon nanotube (CNT)/poly(acrylamide) (GCP@PPy) hydrogel electrodes with a CNT‐free GCP (GP) hydrogel as the electrolyte and chemically soldering an Ag nanowire film to the hydrogel electrode as the current collector. The newly developed dynamic metal‐thiolate (M‐SR, M = Au, Ag) bond‐induced integrated configuration, with an intrinsically powerful electrode and electrolyte, enables the assembled supercapacitor to deliver an areal capacitance of 885 mF cm^?2 and an energy density of 123 µWh cm^?2, which are among the highest‐reported values for stretchable supercapacitors. Notably, the device exhibits a superhigh stretching strain of 800%, rapid optical healing capability, and significant real‐time healability during the charge–discharge process. The exceptional performance combined with the facile assembly method confirms this multifunctional device as the best performer among all the flexible supercapacitors reported to date.     

Stretchable Electronic Sensors of Nanocomposite Network Films for Ultrasensitive Chemical Vapor Sensing

A stretchable, transparent, and body‐attachable chemical sensor is assembled from the stretchable nanocomposite network film for ultrasensitive chemical vapor sensing. The stretchable nanocomposite network film is fabricated by in situ preparation of polyaniline/MoS₂ (PANI/MoS₂) nanocomposite in MoS₂ suspension and simultaneously nanocomposite deposition onto prestrain elastomeric polydimethylsiloxane substrate. The assembled stretchable electronic sensor demonstrates ultrasensitive sensing performance as low as 50 ppb, robust sensing stability, and reliable stretchability for high‐performance chemical vapor sensing. The ultrasensitive sensing performance of the stretchable electronic sensors could be ascribed to the synergistic sensing advantages of MoS₂ and PANI, higher specific surface area, the reliable sensing channels of interconnected network, and the effectively exposed sensing materials. It is expected to hold great promise for assembling various flexible stretchable chemical vapor sensors with ultrasensitive sensing performance, superior sensing stability, reliable stretchability, and robust portability to be potentially integrated into wearable electronics for real‐time monitoring of environment safety and human healthcare.     

An Elastic Autonomous Self‐Healing Capacitive Sensor Based on a Dynamic Dual Crosslinked Chemical System

Adopting self‐healing, robust, and stretchable materials is a promising method to enable next‐generation wearable electronic devices, touch screens, and soft robotics. Both elasticity and self‐healing are important qualities for substrate materials as they comprise the majority of device components. However, most autonomous self‐healing materials reported to date have poor elastic properties, i.e., they possess only modest mechanical strength and recoverability. Here, a substrate material designed is reported based on a combination of dynamic metal‐coordinated bonds (β‐diketone–europium interaction) and hydrogen bonds together in a multiphase separated network. Importantly, this material is able to undergo self‐healing and exhibits excellent elasticity. The polymer network forms a microphase‐separated structure and exhibits a high stress at break (≈1.8 MPa) and high fracture strain (≈900%). Additionally, it is observed that the substrate can achieve up to 98% self‐healing efficiency after 48 h at 25 °C, without the need of any external stimuli. A stretchable and self‐healable dielectric layer is fabricated with a dual‐dynamic bonding polymer system and self‐healable conductive layers are created using polymer as a matrix for a silver composite. These materials are employed to prepare capacitive sensors to demonstrate a stretchable and self‐healable touch pad.     

Flexible and Transparent Gas Molecule Sensor Integrated with Sensing and Heating Graphene Layers

Graphene leading to high surface‐to‐volume ratio and outstanding conductivity is applied for gas molecule sensing with fully utilizing its unique transparent and flexible functionalities which cannot be expected from solid‐state gas sensors. In order to attain a fast response and rapid recovering time, the flexible sensors also require integrated flexible and transparent heaters. Here, large‐scale flexible and transparent gas molecule sensor devices, integrated with a graphene sensing channel and a graphene transparent heater for fast recovering operation, are demonstrated. This combined all‐graphene device structure enables an overall device optical transmittance that exceeds 90% and reliable sensing performance with a bending strain of less than 1.4%. In particular, it is possible to classify the fast (≈14 s) and slow (≈95 s) response due to sp²‐carbon bonding and disorders on graphene and the self‐integrated graphene heater leads to the rapid recovery (≈11 s) of a 2 cm × 2 cm sized sensor with reproducible sensing cycles, including full recovery steps without significant signal degradation under exposure to NO₂ gas.     

Colorless,Transparent, Robust,and Fast Scratch‐Self‐Healing Elastomers via a Phase‐Locked Dynamic Bonds Design

Robust self‐healing thermoplastic elastomers are expected to have repeated healing capability, remarkable mechanical properties, transparency, and superior toughness. The phase‐locked design in this work provides excellent tensile mechanical properties and efficient healability at a moderate temperature due to the dynamic disulfide bonds embedded in the hard segments and mainly being locked in the viscoelastic hard microphase region. The self‐healing elastomers exhibit a maximum tensile stress of 25 MPa and a fracture strain of over 1600%, which are quite prominent compared to previous reports. The nanoscale domains of the elastomer are smaller than the wavelength of visible light by microphase separation control resulting in colorless, nearly 100% transparency, and are as good as quartz glasses. The high dynamics of the phase‐locked disulfide bonds renders a high healing efficiency of scratches on the surface within 60 s at 70 °C. The rapid scratch healing and complete transparency recovery of the elastomers provide new avenues in the highly transparent surface or protective films which finds potential applications for precision optical lenses, flexible display screens, and automobile or aircraft lighting finishes.     

Flexible Transparent Electronic Gas Sensors

Flexible and transparent electronic gas sensors capable of real‐time, sensitive, and selective analysis at room‐temperature, have gained immense popularity in recent years for their potential to be integrated into various smart wearable electronics and display devices. Here, recent advances in flexible transparent sensors constructed from semiconducting oxides, carbon materials, conducting polymers, and their nanocomposites are presented. The sensing material selection, sensor device construction, and sensing mechanism of flexible transparent sensors are discussed in detail. The critical challenges and future development associated with flexible and transparent electronic gas sensors are presented. Smart wearable gas sensors are believed to have great potential in environmental monitoring and noninvasive health monitoring based on disease biomarkers in exhaled gas.     

Microtopography‐Guided Conductive Patterns of Liquid‐Driven Graphene Nanoplatelet Networks for Stretchable and Skin‐Conformal Sensor Array

Flexible thin‐film sensors have been developed for practical uses in invasive or noninvasive cost‐effective healthcare devices, which requires high sensitivity, stretchability, biocompatibility, skin/organ‐conformity, and often transparency. Graphene nanoplatelets can be spontaneously assembled into transparent and conductive ultrathin coatings on micropatterned surfaces or planar substrates via a convective Marangoni force in a highly controlled manner. Based on this versatile graphene assembled film preparation, a thin, stretchable and skin‐conformal sensor array (144 pixels) is fabricated having microtopography‐guided, graphene‐based, conductive patterns embedded without any complicated processes. The electrically controlled sensor array for mapping spatial distributions (144 pixels) shows high sensitivity (maximum gauge factor ≈1697), skin‐like stretchability (<48%), high cyclic stability or durability (over 10⁵ cycles), and the signal amplification (≈5.25 times) via structure‐assisted intimate‐contacts between the device and rough skin. Furthermore, given the thin‐film programmable architecture and mechanical deformability of the sensor, a human skin‐conformal sensor is demonstrated with a wireless transmitter for expeditious diagnosis of cardiovascular and cardiac illnesses, which is capable of monitoring various amplified pulse‐waveforms and evolved into a mechanical/thermal‐sensitive electric rubber‐balloon and an electronic blood‐vessel. The microtopography‐guided and self‐assembled conductive patterns offer highly promising methodology and tool for next‐generation biomedical devices and various flexible/stretchable (wearable) devices.     

A Stretchable and Self‐Healing Energy Storage Device Based on Mechanically and Electrically Restorative Liquid‐Metal Particles and Carboxylated Polyurethane Composites

Stretchable and self‐healing (SH) energy storage devices are indispensable elements in energy‐autonomous electronic skin. However, the current collectors are not self‐healable nor intrinsically stretchable, they mostly rely on strain‐accommodating structures that require complex processing, are often limited in stretchability, and suffer from low device packing density and fragility. Here, an SH conductor comprising nickel flakes, eutectic gallium indium particles (EGaInPs), and carboxylated polyurethane (CPU) is presented. An energy storage device is constructed by the two SH electrodes assembled with graphene nanoplatelets sandwiching an ionic‐liquid electrolyte. An excellent electrochemical healability (94% capacity retention upon restretching at 100% after healing from bifurcation) is unveiled, stemming from the complexation modulated redox behavior of EGaIn in the presence of the ligand bis(trifluoromethanesulfonyl)imide, which enhances the reversible Faradaic reaction of Ga. Self‐healing can be achieved where the damaged regions are electrically restored by the flow of liquid metal and mechanically healing activated by the interfacial hydrogen bonding of CPU with an efficiency of 97.5% can be achieved. The SH conductor has an initial conductivity of 2479 S cm^?1 that attains a high stretchability with 700% strain, it restores 100% stretchability even after breaking/healing with the electrical healing efficiency of 75%.     

Bioinspired Flexible Volatile Organic Compounds Sensor Based on Dynamic Surface Wrinkling with Dual‐Signal Response

Living systems can respond to external stimuli by dynamic interface changes. Moreover, natural wrinkle structures allow the surface to switch dynamically and reversibly from flat to rough in response to specific stimuli. Artificial wrinkle structures have been developed for applications such as optical devices, mechanical sensors, and microfluidic devices. However, chemical molecule‐triggered flexible sensors based on dynamic surface wrinkling have not been demonstrated. Inspired by human skin wrinkling, herein, a volatile organic compound (VOC)‐responsive flexible sensor with a switchable dual‐signal response (transparency and resistance) is achieved based on a multilayered Ag nanowire (AgNW)/SiO_x/polydimethylsiloxane (PDMS) film. Wrinkle structures can form dynamically in response to VOC vapors (such as ethanol, toluene, acetone, formaldehyde, and methanol) due to the instability of the multilayer induced by their different swelling capabilities. By controlling the modulus of PDMS and the thickness of the SiO_x layer, tunable sensitivities in resistance and transparency of the device are achieved. Additionally, the proximity mechanism of the solubility parameter is proposed, which explains the high selectivity of the device toward ethanol vapor compared with that of other VOCs well. This stimuli‐responsive sensor exhibits the dynamic visual feedback and the quantitative electrical signal, which provide a novel approach for developing smart flexible electronics.     

Flexible Transparent and Free‐Standing SiC Nanowires Fabric: Stretchable UV Absorber and Fast‐Response UV‐A Detector

Transparent and flexible materials are desired for the construction of photoelectric multifunctional integrated devices and portable electronics. Herein, 2H‐SiC nanowires are assembled into a flexible, transparent, self‐standing nanowire fabric (FTS‐NWsF). The as‐synthesized ultralong nanowires form high‐quality crystals with a few stacking faults. The optical transmission spectra reveal that FTS‐NWsF absorbs most incident 200–400 nm light, but remains transparent to visible light. A polydimethylsiloxane (PDMS)–SiC fabric–PDMS sandwich film device exhibits stable electrical output even when repeatedly stretched by up to 50%. Unlike previous SiC nanowires in which stacking faults are prevalent, the transparent, stretchable SiC fabric shows considerable photoelectric activity and exhibits a rapid photoresponse (rise and decay time < 30 ms) to 340–400 nm light, covering most of the UV‐A spectral region. These advances represent significant progress in the design of functional optoelectronic SiC nanowires and transparent and stretchable optoelectronic systems.     

Vitrimer Elastomer‐Based Jigsaw Puzzle‐Like Healable Triboelectric Nanogenerator for Self‐Powered Wearable Electronics

Functional polymers possess outstanding uniqueness in fabricating intelligent devices such as sensors and actuators, but they are rarely used for converting mechanical energy into electric power. Here, a vitrimer based triboelectric nanogenerator (VTENG) is developed by embedding a layer of silver nanowire percolation network in a dynamic disulfide bond‐based vitrimer elastomer. In virtue of covalent dynamic disulfide bonds in the elastomer matrix, a thermal stimulus enables in situ healing if broken, on demand reconfiguration of shape, and assembly of more sophisticated structures of VTENG devices. On rupture or external damage, the structural integrity and conductivity of VTENG are restored under rapid thermal stimulus. The flexible and stretchable VTENG can be scaled up akin to jigsaw puzzles and transformed from 2D to 3D structures. It is demonstrated that this self‐healable and shape‐adaptive VTENG can be utilized for mechanical energy harvesters and self‐powered tactile/pressure sensors with extended lifetime and excellent design flexibility. These results show that the incorporation of organic materials into electronic devices can not only bestow functional properties but also provide new routes for flexible device fabrication.     

Continuous Fabrication of Meter‐Scale Single‐Wall Carbon Nanotube Films and their Use in Flexible and Transparent Integrated Circuits

Single‐wall carbon nanotubes (SWCNTs), especially in the form of large‐area and high‐quality thin films, are a promising material for use in flexible and transparent electronics. Here, a continuous synthesis, deposition, and transfer technique is reported for the fabrication of meter‐scale SWCNT thin films, which have an excellent optoelectrical performance including a low sheet resistance of 65 Ω/? with a transmittance of 90% at a wavelength of 550 nm. Using these SWCNT thin films, high‐performance all‐CNT thin‐film transistors and integrated circuits are demonstrated, including 101‐stage ring oscillators. The results pave the way for the future development of large‐scale, flexible, and transparent electronics based on CNT thin films.     

Highly Transparent,Stretchable, and Self‐Healing Ionic‐Skin Triboelectric Nanogenerators for Energy Harvesting and Touch Applications

Recently developed triboelectric nanogenerators (TENGs) act as a promising power source for self‐powered electronic devices. However, the majority of TENGs are fabricated using metallic electrodes and cannot achieve high stretchability and transparency, simultaneously. Here, slime‐based ionic conductors are used as transparent current‐collecting layers of TENG, thus significantly enhancing their energy generation, stretchability, transparency, and instilling self‐healing characteristics. This is the first demonstration of using an ionic conductor as the current collector in a mechanical energy harvester. The resulting ionic‐skin TENG (IS‐TENG) has a transparency of 92% transmittance, and its energy‐harvesting performance is 12 times higher than that of the silver‐based electronic current collectors. In addition, they are capable of enduring a uniaxial strain up to 700%, giving the highest performance compared to all other transparent and stretchable mechanical‐energy harvesters. Additionally, this is the first demonstration of an autonomously self‐healing TENG that can recover its performance even after 300 times of complete bifurcation. The IS‐TENG represents the first prototype of a highly deformable and transparent power source that is able to autonomously self‐heal quickly and repeatedly at room temperature, and thus can be used as a power supply for digital watches, touch sensors, artificial intelligence, and biointegrated electronics.     

Performance Enhancement of Electronic and Energy Devices via Block Copolymer Self‐Assembly

The use of self‐assembled block copolymers (BCPs) for the fabrication of electronic and energy devices has received a tremendous amount of attention as a non‐traditional approach to patterning integrated circuit elements at nanometer dimensions and densities inaccessible to traditional lithography techniques. The exquisite control over the dimensional features of the self‐assembled nanostructures (i.e., shape, size, and periodicity) is one of the most attractive properties of BCP self‐assembly. Harmonic spatial arrangement of the self‐assembled nanoelements at desired positions on the chip may offer a new strategy for the fabrication of electronic and energy devices. Several recent reports show the great promise in using BCP self‐assembly for practical applications of electronic and energy devices, leading to substantial enhancements of the device performance. Recent progress is summarized here, with regard to the performance enhancements of non‐volatile memory, electrical sensor, and energy devices enabled by directed BCP self‐assembly.     

Heterogeneous Integration of Carbon‐Nanotube–Graphene for High‐Performance,Flexible, and Transparent Photodetectors

Low‐dimensional carbon materials, such as semiconducting carbon nanotubes (CNTs), conducting graphene, and their hybrids, are of great interest as promising candidates for flexible, foldable, and transparent electronics. However, the development of highly photoresponsive, flexible, and transparent optoelectronics still remains limited due to their low absorbance and fast recombination rate of photoexcited charges, despite the considerable potential of photodetectors for future wearable and foldable devices. This work demonstrates a heterogeneous, all‐carbon photodetector composed of graphene electrodes and porphyrin‐interfaced single‐walled CNTs (SWNTs) channel, exhibiting high photoresponse, flexibility, and full transparency across the device. The porphyrin molecules generate and transfer photoexcited holes to the SWNTs even under weak white light, resulting in significant improvement of photoresponsivity from negligible to 1.6 × 10^?2 A W^?1. Simultaneously, the photodetector exhibits high flexibility allowing stable light detection under ≈50% strain (i.e., a bending radius of ≈350 µm), and retaining a sufficient transparency of ≈80% at 550 nm. Experimental demonstrations as a wearable sunlight sensor highlight the utility of the photodetector that can be conformally mounted on human skin and other curved surfaces without any mechanical and optical constraints. The heterogeneous integration of porphyrin–SWNT–graphene may provide a viable route to produce invisible, high‐performance optoelectronic systems.     

Superior Toughness and Fast Self‐Healing at Room Temperature Engineered by Transparent Elastomers

The most important properties of self‐healing polymers are efficient recovery at room temperature and prolonged durability. However, these two characteristics are contradictory, making it difficult to optimize them simultaneously. Herein, a transparent and easily processable thermoplastic polyurethane (TPU) with the highest reported tensile strength and toughness (6.8 MPa and 26.9 MJ m^?3, respectively) is prepared. This TPU is superior to reported contemporary room‐temperature self‐healable materials and conveniently heals within 2 h through facile aromatic disulfide metathesis engineered by hard segment embedded aromatic disulfides. After the TPU film is cut in half and respliced, the mechanical properties recover to more than 75% of those of the virgin sample within 2 h. Hard segments with an asymmetric alicyclic structure are more effective than those with symmetric alicyclic, linear aliphatic, and aromatic structures. An asymmetric structure provides the optimal metathesis efficiency for the embedded aromatic disulfide while preserving the remarkable mechanical properties of TPU, as indicated by rheological and surface investigations. The demonstration of a scratch‐detecting electrical sensor coated on a tough TPU film capable of auto‐repair at room temperature suggests that this film has potential applications in the wearable electronics industry.     

Fabrication of Flexible MoS2 Thin‐Film Transistor Arrays for Practical Gas‐Sensing Applications

By combining two kinds of solution‐processable two‐dimensional materials, a flexible transistor array is fabricated in which MoS₂ thin film is used as the active channel and reduced graphene oxide (rGO) film is used as the drain and source electrodes. The simple device configuration and the 1.5 mm‐long MoS₂ channel ensure highly reproducible device fabrication and operation. This flexible transistor array can be used as a highly sensitive gas sensor with excellent reproducibility. Compared to using rGO thin film as the active channel, this new gas sensor exhibits much higher sensitivity. Moreover, functionalization of the MoS₂ thin film with Pt nanoparticles further increases the sensitivity by up to ～3 times. The successful incorporation of a MoS₂ thin‐film into the electronic sensor promises its potential application in various electronic devices.     

Extraordinarily Stretchable All‐Carbon Collaborative Nanoarchitectures for Epidermal Sensors

Multifunctional microelectronic components featuring large stretchability, high sensitivity, high signal‐to‐noise ratio (SNR), and broad sensing range have attracted a huge surge of interest with the fast developing epidermal electronic systems. Here, the epidermal sensors based on all‐carbon collaborative percolation network are demonstrated, which consist 3D graphene foam and carbon nanotubes (CNTs) obtained by two‐step chemical vapor deposition processes. The nanoscaled CNT networks largely enhance the stretchability and SNR of the 3D microarchitectural graphene foams, endowing the strain sensor with a gauge factor as high as 35, a wide reliable sensing range up to 85%, and excellent cyclic stability (>5000 cycles). The flexible and reversible strain sensor can be easily mounted on human skin as a wearable electronic device for real‐time and high accuracy detecting of electrophysiological stimuli and even for acoustic vibration recognition. The rationally designed all‐carbon nanoarchitectures are scalable, low cost, and promising in practical applications requiring extraordinary stretchability and ultrahigh SNRs.