Self-Healing,Robust, and Stretchable Electrode by Direct Printing on Dynamic Polyurea Surface at Slightly Elevated Temperature

Printed electronics on elastomer substrates have found wide applications in wearable devices and soft robotics. For everyday usage, additional requirements exist for the robustness of the printed flexible electrodes, such as the ability to resist scratching and damage. Therefore, highly robust electrodes with self-healing, and good mechanical strength and stretchability are highly required and challenging. In this paper, a cross-linking polyurea using polydimethylsiloxane as the soft segment and dynamic urea bonds is prepared and serves as a self-healing elastomer substrate for coating and printing of silver nanowires (AgNWs). Due to the dynamic exchangeable urea bond at 60 °C, the elastomer exhibits dynamic exchange of the cross-linking network while retaining the macroscopic shape. As a result, the AgNWs are partially embedded in the surface of the elastomer substrate when coated or printed at 60 °C, forming strong interfacial adhesion. As a result, the obtained stretchable electrode exhibits high mechanical strength and stretchability, the ability to resist scratching and sonication, and self-healing. This strategy can be applied to a variety of different conducting electrode materials including AgNWs, silver particles, and liquid metal, which provides a new way to prepare robust and self-healing printed electronics.     

Environment Tolerant Conductive Nanocomposite Organohydrogels as Flexible Strain Sensors and Power Sources for Sustainable Electronics

Conductive hydrogels (CHs) have been highlighted in the design of flexible strain sensors and stretchable triboelectric nanogenerators (TENGs) on the basis of their excellent physicochemical properties such as large stretchability and high conductivity. Nevertheless, the incident freezing and drying behaviors of CHs by using water solvent as the dispersion medium limit their application scopes significantly. Herein, an environment tolerant and ultrastretchable organohydrogel is demonstrated by a simple solvent-replacement strategy, in which the partial water in the as-synthesized polyacrylamide/montmorillonite/carbon nanotubes hydrogel is replaced with the glycerol, leading to excellent temperature toleration (−60 to 60 °C) and good stability (30 days under normal environment) without sacrificing the stretchability and conductivity. The organohydrogel exhibits an ultrawide strain sensing range (0–4196%) with a high sensitivity of 8.5, enabling effective detection and discrimination of human activities that are gentle or drastic under various conditions. Furthermore, the organohydrogel is assembled in a single-electrode TENG, which displays excellent energy harvesting ability even under a stretchability of 500% and robustness to directly power wearable electronics in harsh cold conditions. This work inspires a simple route for multifunctional organohydrogel and promises the practical application of flexible and self-powered wearable devices in extreme environments.     

Coaxial Thermoplastic Elastomer‐Wrapped Carbon Nanotube Fibers for Deformable and Wearable Strain Sensors

Highly conductive and stretchable fibers are crucial components of wearable electronics systems. Excellent electrical conductivity, stretchability, and wearability are required from such fibers. Existing technologies still display limited performances in these design requirements. Here, achieving highly stretchable and sensitive strain sensors by using a coaxial structure, prepared via coaxial wet spinning of thermoplastic elastomer‐wrapped carbon nanotube fibers, is proposed. The sensors attain high sensitivity (with a gauge factor of 425 at 100% strain), high stretchability, and high linearity. They are also reproducible and durable. Their use as safe sensing components on deformable cable, expandable surfaces, and wearable textiles is demonstrated.     

Flexible Electronics: Stretchable Electrodes and Their Future

Flexible electronics, as an emerging and exciting research field, have brought great interest to the issue of how to make flexible electronic materials that offer both durability and high performance at strained states. With the advent of on‐body wearable and implantable electronics, as well as increasing demands for human‐friendly intelligent soft robots, enormous effort is being expended on highly flexible functional materials, especially stretchable electrodes, by both the academic and industrial communities. Among different deformation modes, stretchability is the most demanding and challenging. This review focuses on the latest advances in stretchable transparent electrodes based on a new design strategy known as kirigami (the art of paper cutting) and investigates the recent progress on novel applications, including skin‐like electronics, implantable biodegradable devices, and bioinspired soft robotics. By comparing the optoelectrical and mechanical properties of different electrode materials, some of the most important outcomes with comments on their merits and demerits are raised. Key design considerations in terms of geometries, substrates, and adhesion are also discussed, offering insights into the universal strategies for engineering stretchable electrodes regardless of the material. It is suggested that highly stretchable and biocompatible electrodes will greatly boost the development of next‐generation intelligent life‐like electronics.     

Self‐Healable and Stretchable Organic Thermoelectric Materials: Electrically Percolated Polymer Nanowires Embedded in Thermoplastic Elastomer Matrix

Self‐healable and stretchable energy‐harvesting materials can provide a new avenue for the realization of self‐powered wearable electronics, including electronic skins, whose main materials are required to be robust to and stable under external damage and severe mechanical stresses. However, thermoelectric (TE) materials showing both self‐healing properties and stretchability have not yet been demonstrated despite their great potential to harvest thermal energy in the human body. As most existing TE materials are either mechanically brittle or unrecoverable after being subjected to damage, a novel approach is necessary for designing such materials. Herein, self‐healable and stretchable TE materials based on all‐organic composite system wherein polymer semiconductor nanowires are p‐doped with a molecular dopant and embedded in a thermoplastic elastomer matrix are reported. The polymer nanowires are electrically percolated in the matrix, and the resulting composite materials exhibit good TE performance. The composites also exhibit both excellent self‐healing properties under mild heat and pressure conditions and good stretchability. It is believed that this work can be a cornerstone for the design of self‐healable and stretchable energy‐harvesting materials as it provides useful guidelines for imparting electrical conductivity to insulating thermoplastic elastomers, which typically possess versatile and useful mechanical properties.     

3D Interconnected Conductive Graphite Nanoplatelet Welded Carbon Nanotube Networks for Stretchable Conductors

Stretchable conductors with stable electrical conductivity under harsh mechanical deformations are essential for developing next generation portable and flexible wearable electronics. To achieve both high stretchability and conductivity with electromechanical stability, highly stretchable conductors based on 3D interconnected conductive graphite nanoplatelet welded carbon nanotube (GNP-w-CNT) networks are fabricated by welding the junctions of CNTs using GNPs followed by infiltrating with poly(dimethylsiloxane) (PDMS). It is observed that GNPs can weld the adjacent CNTs to facilitate the formation of continuous conductive pathways and avoid interfacial slippage under repetitive stretching. The enhanced interfacial bonding enables the conductor both high electrical conductivity (>132 S m⁻¹) and high stretchability (>150% strain) while ensuring long-term stability (1000 stretching-releasing cycles under 60% tensile strain). To demonstrate the outstanding flexibility and electrical stability, a flexible and stretchable light-emitting diode circuit with stable performance during stretching, bending, twisting, and pressing conditions is further fabricated. The unique welding mechanism can be easily extended to other material systems to broaden the application of stretchable conductors to a myriad of new applications.     

Stretchable Electrode Based on Laterally Combed Carbon Nanotubes for Wearable Energy Harvesting and Storage Devices

Carbon nanotubes (CNTs) are a promising material for use as a flexible electrode in wearable energy devices due to their electrical conductivity, soft mechanical properties, electrochemical activity, and large surface area. However, their electrical resistance is higher than that of metals, and deformations such as stretching can lead to deterioration of electrical performances. To address these issues, here a novel stretchable electrode based on laterally combed CNT networks is presented. The increased percolation between combed CNTs provides a high electrical conductivity even under mechanical deformations. Additional nickel electroplating and serpentine electrode designs increase conductivity and deformability further. The resulting stretchable electrode exhibits an excellent sheet resistance, which is comparable to conventional metal film electrodes. The resistance change is minimal even when stretched by ≈100%. Such high conductivity and deformability in addition to intrinsic electrochemically active property of CNTs enable high performance stretchable energy harvesting (wireless charging coil and triboelectric generator) and storage (lithium ion battery and supercapacitor) devices. Monolithic integration of these devices forms a wearable energy supply system, successfully demonstrating its potential as a novel soft power supply module for wearable electronics.     

Stretchable,Transparent, and Thermally Stable Triboelectric Nanogenerators Based on Solvent‐Free Ion‐Conducting Elastomer Electrodes

The development of stretchable/soft electronics requires power sources that can match their stretchability. In this study, a highly stretchable, transparent, and environmentally stable triboelectric nanogenerator with ionic conductor electrodes (iTENG) is reported. The ion‐conducting elastomer (ICE) electrode, together with a dielectric elastomer electrification layer, allows the ICE‐iTENG to achieve a stretchability of 1036% and transmittance of 91.5%. Most importantly, the ICE is liquid solvent‐free and thermally stable up to 335 °C, avoiding the dehydration‐induced performance degradation of commonly used hydrogels. The ICE‐iTENG shows no decrease in electrical output even after storing at 100 °C for 15 h. Biomechanical motion energies are demonstrated to be harvested by the ICE‐iTENG for powering wearable electronics intermittently without extra power sources. An ICE‐iTENG‐based pressure sensor is also developed with sensitivity up to 2.87 kPa^?1. The stretchable ICE‐iTENG overcomes the strain‐induced performance degradation using percolated electrical conductors and liquid evaporation‐induced degradation using ion‐conducting hydrogels/ionogels, suggesting great promising applications in soft/stretchable electronics under a relatively wider temperature range.     

Tough,Bio-disintegrable and Stretchable Substrate Reinforced with Nanofibers for Transient Wearable Electronics

Research on transient wearable electronics with stretchable components is of increasing interest because of their abilities to conform seamlessly to human tissues and, more interestingly, disappear from the environment when disposed. To wear them comfortably, their component materials must be pliable, tough, stretchable, biocompatible, and disintegrable. However, most biodegradable materials are not stretchable or tough, limiting their use in transient wearable electronics. Herein, these challenges are addressed by demonstrating a biodegradable nanofiber (NF)-reinforced water-borne polyurethane (NFR-WPU) with stretchability, toughness, and partial biodegradability by embedding biodegradable composite NFs of poly(glycerol sebacate): poly(vinyl alcohol) (PGS:PVA) into the WPU matrix, thus rendering its properties tunable. An optimal loading amount of NFs into the NFR-WPU significantly enhanced the toughness by 19 times while maintaining the Young's modulus as low as 3.3 MPa. Furthermore, the NFR-WPU substrate has very high fracture toughness and shows excellent biocompatibility. Moreover, the NFR-WPU has a disintegration rate nine times greater than that of pristine WPU. Finally, disintegrable and stretchable triboelectric and capacitive touch sensors on the NFR-WPU are fabricated and demonstrated for potential use in transient wearable electronics.     

Metal-Organic Framework Reinforced Highly Stretchable and Durable Conductive Hydrogel-Based Triboelectric Nanogenerator for Biomotion Sensing and Wearable Human-Machine Interfaces

Flexible triboelectric nanogenerators (TENGs) with multifunctional sensing capabilities offer an elegant solution to address the growing energy supply challenges for wearable smart electronics. Herein, a highly stretchable and durable electrode for wearable TENG is developed using ZIF-8 as a reinforcing nanofiller in a hydrogel with LiCl electrolyte. ZIF-8 nanocrystals improve the hydrogel's mechanical properties by forming hydrogen bonds with copolymer chains, resulting in 2.7 times greater stretchability than pure hydrogel. The hydrogel electrode is encapsulated by microstructured silicone layers that act as triboelectric materials and prevent water loss from the hydrogel. Optimized ZIF-8-based hydrogel electrodes enhance the output performance of TENG through the dynamic balance of electric double layers (EDLs) during contact electrification. Thus, the as-fabricated TENG delivers an excellent power density of 3.47 Wm^–2, which is 3.2 times higher than pure hydrogel-based TENG. The developed TENG can scavenge biomechanical energy even at subzero temperatures to power small electronics and serve as excellent self-powered pressure sensors for human-machine interfaces (HMIs). The nanocomposite hydrogel-based TENG can also function as a wearable biomotion sensor, detecting body movements with high sensitivity. This study demonstrates the significant potential of utilizing ZIF-8 reinforced hydrogel as an electrode for wearable TENGs in energy harvesting and sensor technology.     

Strain-Tolerant,High-Detectivity,and Intrinsically Stretchable All-Polymer Photodiodes

A skin-like photodiode (PD) that is stretchable and skin-conformable is crucial to opening the next-generation wearable electronics for optical biometric monitoring, biomedical imaging, and others. To achieve reliable PD characteristics under large deformation, stretchable PDs with high detectivity and high mechanical stretchability must be developed. Herein, intrinsically stretchable polymer-based PDs (is-PPDs) comprising all-polymeric constituent layers are demonstrated. In particular, elastomeric photoactive layers consisting of an elastomer with p-/n-type semiconducting polymers and conducting polymer-based stretchable transparent electrodes with modulated work functions improve both the mechanical stability and the detectivity (D*) of is-PPDs. Accordingly, is-PPDs show excellent D* over 10¹³ Jones with a suppressed dark current density of 0.1 nA cm⁻² before and after 100% stretching. The proposed is-PPDs record high-quality and stable photoplethysmography signals at the wrist with outward extension.     

Paper with Power: Engraving 2D Materials on 3D Structures for Printed,High‐Performance,Binder‐Free,and All‐Solid‐State Supercapacitors

The prevalence of the Internet of Things (IoT) and wearable electronics create an unprecedented demand for new power sources which are low cost, high performance, and flexible in many application settings. In this paper, a strategy for the scalable fabrication of high‐performance, all‐solid‐state supercapacitors (SCs) is demonstrated using conventional paper and an inkjet printer. Emerging printed electronics technology and low‐cost chemical engraving methods are bridged for the first time to construct Cu_xO nanosheets, in situ, on the 3D metallized fiber structures. Benefitting from both the “2D Materials on 3D Structures” design and the binder‐free nature of the fabricated electrodes, substantial improvements to electrical conductivity, aerial capacitance, and electrochemical performance of the resulting SCs are observed. With the proposed strategy, the fabricated SCs can be seamlessly integrated into any printed circuit, sensors, or artwork; the properties of these SCs can be easily tuned by simple pattern design, fulfilling the increasing demand of highly customized power systems in the IoT and flexible/wearable electronics industries.     

Intrinsically Stretchable Organic Solar Cells beyond 10% Power Conversion Efficiency Enabled by Transfer Printing Method

Stretchable organic solar cells (OSCs) simultaneously possessing high-efficiency and robust mechanical properties are ideal power generators for the emerging wearable and portable electronics. Herein, after incorporating a low amount of trimethylsiloxy terminated polydimethylsiloxane (PDMS) additive, the intrinsic stretchability of PTB7-Th:IEICO-4F bulk heterojunction (BHJ) film is greatly improved from 5% to 20% strain without sacrificing the photovoltaic performance. The intimate multi-layers stacking of OSCs is also realized with the transfer printing method assisted by electrical adhesive “glue” D-Sorbitol. The resultant devices with 84% electrode transmittance exhibit a remarkable power conversion efficiency (PCE) of 10.1%, which is among the highest efficiency for intrinsically stretchable OSCs to date. The stretchable OSCs also demonstrate the ultra-flexibility, stretchability, and mechanical robustness, which keep the PCE almost unchanged at small bending radium of 2 mm for 300 times bending cycles and retain 86.7% PCE under tensile strain as large as 20% for the devices with 70% electrode transmittance. The results provide a universal method to fabricate highly efficient intrinsically stretchable OSCs.     

High-Throughput Screening of Self-Healable Polysulfobetaine Hydrogels and their Applications in Flexible Electronics

Hydrogels are promising materials in the applications of wound adhesives, wearable electronics, tissue engineering, implantable electronics, etc. The properties of a hydrogel rely strongly on its composition. However, the optimization of hydrogel properties has been a big challenge as increasing numbers of components are added to enhance and synergize its mechanical, biomedical, electrical, and self-healable properties. Here in this work, it is shown that high-throughput screening can efficiently and systematically explore the effects of multiple components (at least eight) on the properties of polysulfobetaine hydrogels, as well as provide a useful database for diverse applications. The optimized polysulfobetaine hydrogels that exhibit outstanding self-healing and mechanical properties, have been obtained by high-throughput screening. By compositing with poly(3,4-ethylenedioxythiophene):polystyrene sulfonate (PEDOT:PSS), intrinsically self-healable and stretchable conductors are achieved. It is further demonstrated that a polysulfobetaine hydrogel-based electronic skin, which exhibits exceptionally fast self-healing capability of the whole device at ambient conditions. This work successfully extends high-throughput synthetic methodology to the field of hydrogel electronics, as well as demonstrates new directions of healable flexible electronic devices in terms of material development and device design.     

Fluid-Dynamics-Processed Highly Stretchable,Conductive, and Printable Graphene Inks for Real-Time Monitoring Sweat during Stretching Exercise

With the development of wearable electronics, the use of engineered functional inks with printing technologies has attracted attention owing to its potential for applications in low-cost, high-throughput, and high-performance devices. However, the improvement in conductivity and stretchability in the mass production of inks is still a challenge for practical use in wearable applications. Herein, a scalable and efficient fluid dynamics process that produces highly stretchable, conductive, and printable inks containing a high concentration of graphene is reported. The resulting inks, in which the uniform incorporation of exfoliated graphene flakes into a viscoelastic thermoplastic polyurethane is employed, facilitated the screen-printing process, resulting in high conductivity and excellent electromechanical stability. The electrochemical analysis of a stretchable sodium ion sensor based on a serpentine-structured pattern results in excellent electrochemical sensing performance even under strong fatigue tests performed by repeated stretching (300% strain) and release cycles. To demonstrate the practical use of the proposed stretchable conductor, on-body tests are carried out in real-time to monitor the sweat produced by a volunteer during simultaneous physical stretching and stationary cycling. These functional graphene inks have attractive performance and offer exciting potential for a wide range of flexible and wearable electronic applications.     

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.     

Engineering Route for Stretchable, 3D Microarchitectures of Wide Bandgap Semiconductors for Biomedical Applications

Wide bandgap (WBG) semiconductors have attracted significant research interest for the development of a broad range of flexible electronic applications, including wearable sensors, soft logical circuits, and long-term implanted neuromodulators. Conventionally, these materials are grown on standard silicon substrates, and then transferred onto soft polymers using mechanical stamping processes. This technique can retain the excellent electrical properties of wide bandgap materials after transfer and enables flexibility; however, most devices are constrained by 2D configurations that exhibit limited mechanical stretchability and morphologies compared with 3D biological systems. Herein, a stamping-free micromachining process is presented to realize, for the first time, 3D flexible and stretchable wide bandgap electronics. The approach applies photolithography on both sides of free-standing nanomembranes, which enables the formation of flexible architectures directly on standard silicon wafers to tailor the optical transparency and mechanical properties of the material. Subsequent detachment of the flexible devices from the support substrate and controlled mechanical buckling transforms the 2D precursors of wide band gap semiconductors into complex 3D mesoscale structures. The ability to fabricate wide band gap materials with 3D architectures that offer device-level stretchability combined with their multi-modal sensing capability will greatly facilitate the establishment of advanced 3D bio-electronics interfaces.     

Highly Stretchable Bilayer Lattice Structures That Elongate via In‐Plane Deformation

Many emerging technologies such as wearable batteries and electronics require stretchable functional structures made from intrinsically less deformable materials. The stretch capability of most demonstrated stretchable structures often relies on either initially out‐of‐plane configurations or the out‐of‐plane deflection of planar patterns. Such nonplanar features may dramatically increase the surface roughness, cause poor adhesion and adverse effects on subsequent multilayer processing, thereby posing a great challenge for flexible devices that require smooth surfaces (e.g., transparent electrodes in which flat‐surface‐enabled high optical transmittance is preferred). Inspired by the lamellar layouts of collagenous tissues, this work demonstrates a planar bilayer lattice structure, which can elongate substantially via only in‐plane motion and thus maintain a smooth surfaces. The constructed bilayer lattice exhibits a large stretchability up to 360%, far beyond the inherent deformability of the brittle constituent material and comparable to that of state‐of‐the‐art stretchable structures for flexible electronics. A stretchable conductor employing the bilayer lattice designs can remain electrically conductive at a strain of 300%, demonstrating the functionality and potential applications of the bilayer lattice structure. This design opens a new avenue for the development of stretchable structures that demand smooth surfaces.     

Recent Advancements and Perspectives of Biodegradable Polymers for Supercapacitors

Supercapacitors (SCs) have demonstrated great potential for integration into future wearable and implantable electronics, yet the insufficient environmental adaption and biosafety limit their further development. To this regard, application of biodegradable polymers is considered as an ideal solution strategy for the environmentally sound disposal of SCs. The biodegradable polymers with satisfactory degradability and excellent biocompatibility demonstrate an irreplaceable role in the future development of SCs and provide an ideal solution strategy for its environmentally sound disposal. In this review, the research progress and challenges of biodegradable polymers in the field of SCs are discussed and analyzed. First, the classification of existing biodegradable polymers and their typical structure, properties, and preparation processes are elucidated. Subsequently, the main applications of biodegradable polymers in different components of SCs, including electrodes, electrolytes, substrate, and encapsulation materials, are summarized. In addition, the research progress of biodegradable polymer-based SCs in terms of preparation strategies and modification methods is summarized, and the key role of biodegradable polymers in the development process of green SCs is deeply discussed. Finally, the future perspectives and challenges faced by the biodegradable polymer-based SCs are briefly proposed.     

Stretchable and Self-Healable Semiconductive Composites Based on Hydrogen Bonding Cross-linked Elastomeric Matrix

Semiconductors with both high stretchability and self-healing capability are highly desirable for various wearable devices. Much progress has been achieved in designing highly stretchable semiconductive polymers or composites. The demonstration of self-healable semiconductive composite is still rare. Here, an extremely soft, highly stretchable, and self-healable hydrogen bonding cross-linked elastomer, amide functionalized-polyisobutylene (PIB-amide) is developed, to enable a self-healable semiconductive composite through compounding with a high-performance conjugated diketopyrrolopyrrole (DPP-T) polymer. The composite, consisting of 20% DPP-T and 80% PIB-amide, shows record high crack-onset strain (COS ≈1500%), extremely low elastic modulus (E≈1.6 MPa), and unique ability to spontaneously self-heal atroom temperature within 5 min. Unlike previous works, these unique composite materials also show strain-independent charge mobility. An in-depth morphological study based on multi-model techniques indicate that all composites show blending ratio- and stretching-independent fibril-like aggregation due to the strong hydrogen bond in elastomer to enable the unique stable charge mobility. This study provides a new direction to develop highly healable and electronically stable semiconductive composite and will enable new applications of stretchable electronics.