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.     

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.     

Functionally Antagonistic Hybrid Electrode with Hollow Tubular Graphene Mesh and Nitrogen‐Doped Crumpled Graphene for High‐Performance Ionic Soft Actuators

Ionic soft actuators, which exhibit large mechanical deformations under low electrical stimuli, are attracting attention in recent years with the advent of soft and wearable electronics. However, a key challenge for making high‐performance ionic soft actuators with large bending deformation and fast actuation speed is to develop a stretchable and flexible electrode having high electrical conductivity and electrochemical capacitance. Here, a functionally antagonistic hybrid electrode with hollow tubular graphene meshes and nitrogen‐doped crumpled graphene is newly reported for superior ionic soft actuators. Three‐dimensional network of hollow tubular graphene mesh provides high electrical conductivity and mechanically resilient functionality on whole electrode domain. On the contrary, nitrogen‐doped wrinkled graphene supplies ultrahigh capacitance and stretchability, which are indispensably required for improving electrochemical activity in ionic soft actuators. Present results show that the functionally antagonistic hybrid electrode greatly enhances the actuation performances of ionic soft actuators, resulting in much larger bending deformation up to 620%, ten times faster rise time and much lower phase delay in a broad range of input frequencies. This outstanding enhancement mostly attributes to exceptional properties and synergistic effects between hollow tubular graphene mesh and nitrogen‐doped crumpled graphene, which have functionally antagonistic roles in charge transfer and charge injection, respectively.     

Room‐Temperature Nanosoldering of a Very Long Metal Nanowire Network by Conducting‐Polymer‐Assisted Joining for a Flexible Touch‐Panel Application

As an alternative to the brittle and expensive indium tin oxide (ITO) transparent conductor, a very simple, room‐temperature nanosoldering method of Ag nanowire percolation network is developed with conducting polymer to demonstrate highly flexible and even stretchable transparent conductors. The drying conducting polymer on Ag nanowire percolation network is used as a nanosoldering material inducing strong capillary‐force‐assisted stiction of the nanowires to other nanowires or to the substrate to enhance the electrical conductivity, mechanical stability, and adhesion to the substrate of the nanowire percolation network without the conventional high‐temperature annealing step. Highly bendable Ag nanowire/conducting polymer hybrid films with low sheet resistance and high transmittance are demonstrated on a plastic substrate. The fabricated flexible transparent electrode maintains its conductivity over 20 000 cyclic bends and 5 to 10% stretching. Finally, a large area (A4‐size) transparent conductor and a flexible touch panel on a non‐flat surface are fabricated to demonstrate the possibility of cost‐effective mass production as well as the applicability to the unconventional arbitrary soft surfaces. These results suggest that this is an important step toward producing intelligent and multifunctional soft electric devices as friendly human/electronics interface, and it may ultimately contribute to the applications in wearable computers.     

Liquid Metal Based Island‐Bridge Architectures for All Printed Stretchable Electrochemical Devices

The adoption of epidermal electronics into everyday life requires new design and fabrication paradigms, transitioning away from traditional rigid, bulky electronics towards soft devices that adapt with high intimacy to the human body. Here, a new strategy is reported for fabricating achieving highly stretchable “island‐bridge” (IB) electrochemical devices based on thick‐film printing process involving merging the deterministic IB architecture with stress‐enduring composite silver (Ag) inks based on eutectic gallium‐indium particles (EGaInPs) as dynamic electrical anchors within the inside the percolated network. The fabrication of free‐standing soft Ag‐EGaInPs‐based serpentine “bridges” enables the printed microstructures to maintain mechanical and electrical properties under an extreme (≈800%) strain. Coupling these highly stretchable “bridges” with rigid multifunctional “island” electrodes allows the realization of electrochemical devices that can sustain high mechanical deformation while displaying an extremely attractive and stable electrochemical performance. The advantages and practical utility of the new printed Ag‐liquid metal‐based island‐bridge designs are discussed and illustrated using a wearable biofuel cell. Such new scalable and tunable fabrication strategy will allow to incorporate a wide range of materials into a single device towards a wide range of applications in wearable electronics.     

Conductive Hydrogel-Based Electrodes and Electrolytes for Stretchable and Self-Healable Supercapacitors

Stretchable self-healing supercapacitors (SCs) can operate under extreme deformation and restore their initial properties after damage with considerably improved durability and reliability, expanding their opportunities in numerous applications, including smart wearable electronics, bioinspired devices, human–machine interactions, etc. It is challenging, however, to achieve mechanical stretchability and self-healability in energy storage technologies, wherein the key issue lies in the exploitation of ideal electrode and electrolyte materials with exceptional mechanical stretchability and self-healing ability besides conductivity. Conductive hydrogels (CHs) possess unique hierarchical porous structure, high electrical/ionic conductivity, broadly tunable physical and chemical properties through molecular design and structure regulation, holding tremendous promise for stretchable self-healing SCs. Hence, this review is innovatively constructed with a focus on stretchable and self-healing CH based electrodes and electrolytes for SCs. First, the common synthetic approaches of CHs are introduced; then the stretching and self-healing strategies involved in CHs are systematically elaborated; followed by an explanation of the conductive mechanism of CHs; then focusing on CH-based electrodes and electrolytes for stretchable self-healing SCs; subsequently, application of stretchable and self-healing SCs in wearable electronics are discussed; finally, a conclusion is drawn along with views on the challenges and future research directions regarding the field of CHs for SCs.     

Conductive PEDOT:PSS on surface-functionalized chitosan biopolymers for stretchable skin-like electronics

Poly(3,4-ethylenedioxythiophene):poly(styrenesulfonate) (PEDOT:PSS) is a promising alternative transparent electrode to replace conventional indium tix oxide (ITO) for flexible and stretchable electronics. For their applications in optoelectronic devices, realizing both high conductivity and transmittance for the films is of great necessity as a suitable high performance transparent electrode. Here, we demonstrate simultaneously enhanced electrical and optical properties of PEDOT:PSS films prepared on chitosan bio-substrates by using an organic surface modifier, 11-aminoundecanoic acid (11-AA). The sheet resistance of PEDOT:PSS films decreases from 1120.8 to 292.8 Ω/sq with an increase in a transmittance from 75.9 to 80.4% by 11-AA treatment on the chitosan films. The functional groups of 11-AA effectively enhance the adhesion property at the interface between the chitosan substrate and PEDOT:PSS by forming strong interfacial bondings and decrease insulating PSS from PEDOT:PSS films. The wearable heater devices and on-skin sensors based on the 11-AA-treated PEDOT:PSS on the chitosan bio-substrates are successfully fabricated, showing the excellent thermal and sensing performances. The 11-AA surface-modification approach for highly conductive PEDOT:PSS on chitosan bio-substrates presents a great potential for applications toward transparent, flexible and stretchable electronics.     

Design Criteria for Horseshoe and Spiral-Based Interconnects for Highly Stretchable Electronic Devices

Stretchable electronics can be used for numerous advanced applications such as soft and wearable actuators, sensors, bio-implantable devices, and surgical tools because of their ability to conform to curvilinear surfaces, including human skin. The efficacy of these devices depends on the development of stretchable geometries such as interconnection-based configurations and the associated mechanics that helps to achieve optimum configurations. This work presents the essential mechanics of silicon (Si) island-interconnection structures, which include horseshoe and spiral interconnections, without reducing the areal efficiency. In particular, this study demonstrates the range of the geometrical parameters where they have a high stretchability and cyclic life. The numerical results predict the areas that are prone to breaking followed by experimental validation. The figure-of-merit for these configurations is achieved by mapping the fracture-free zones for in-plane and out-of-plane stretching with essential implications in stretchable and wearable system design. Furthermore, this work demonstrates the mechanical response for a range of materials (i.e., copper, gold, aluminum, silver, and graphene) that experience the plastic deformations in contrast to conventionally used Si-based devices that represent the extended usage for advanced stretchable electronic devices. The detailed mechanics of these configurations provides comprehensive guidelines to manufacture wearable and stretchable electronic devices.     

Optically Transparent and Mechanically Robust Ionic Hydrogel Electrodes for Bright Electroluminescent Devices Achieving High Stretchability Over 1400%

To realize wearable displays and interactive soft robots, significant research efforts are focused on developing highly deformable alternating-current electroluminescent (ACEL) devices. Although soft emission layers are well developed, designing stretchable, conductive, and transparent soft electrodes remains challenging. In this study, ionic hydrogels are prepared comprising a double network (DN) of poly(N-hydroxyethylacrylamide-co-acrylamide)/crosslinked chitosan swollen in aqueous lithium bis(trifluoromethanesulfonyl) imide. Owing to the finely tuned DN structure of the polymeric crosslinker and transparent electrolyte, the developed ionic hydrogels exhibit remarkable stretchability (1400%), excellent optical transmittance (>99%), and high conductivity (1.95 × 10⁻² Sm⁻¹). Based on the high performance of the ionic hydrogels, ACEL devices are fabricated with an emission layer containing phosphor microparticles and demonstrate stable, high luminance under extreme deformation, and ultra-high elongation. The excellent transparency of the ionic hydrogel further enables the fabrication of novel soft ACEL devices with tandem structures by stacking several emission and electrode layers, in which each emission layer is independently controlled with a switch circuit.     

Wearable Energy Generating and Storing Textile Based on Carbon Nanotube Yarns

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

Advances on Emerging Materials for Flexible Supercapacitors: Current Trends and Beyond

The progressive size reduction of electronic components is experiencing bottlenecks in shrinking charge storage devices like batteries and supercapacitors, limiting their development into wearable and flexible zero‐pollution technologies. The inherent long cycle life, rapid charge–discharge patterns, and power density of supercapacitors rank them superior over other energy storage devices. In the modern market of zero‐pollution energy devices, currently the lightweight formula and shape adaptability are trending to meet the current requirement of wearables. Carbon nanomaterials have the potential to meet this demand, as they are the core of active electrode materials for supercapacitors and texturally tailored to demonstrate flexible and stretchable properties. With this perspective, the latest progress in novel materials from conventional carbons to recently developed and emerging nanomaterials toward lightweight stretchable active compounds for flexi‐wearable supercapacitors is presented. In addition, the limitations and challenges in realizing wearable energy storage systems and integrating the future of nanomaterials for efficient wearable technology are provided. Moreover, future perspectives on economically viable materials for wearables are also discussed, which could motivate researchers to pursue fabrication of cheap and efficient flexible nanomaterials for energy storage and pave the way for enabling a wide‐range of material‐based applications.     

Highly Stretchable and Strain-Insensitive Liquid Metal based Elastic Kirigami Electrodes (LM-eKE) (Adv. Funct. Mater. 30/2023)

Kirigami, a traditional paper-cutting art, is a promising method for creating mechanically robust circuitry for unconventional devices capable of extreme stretchability through structural deformation. In this study, this design approach is expanded upon by introducing Liquid Metal based Elastic Kirigami Electrodes (LM-eKE) in which kirigami-patterned soft elastomers are coated with eutectic gallium-indium (EGaIn) alloy. Overcoming the mechanical and electrical limitations of previous efforts with paper-like kirigami, the all soft LM-eKE can be stretched to 820% strain while the electrical resistance only increases by 33%. This is enabled by the fluidic properties of the EGaIn coating, which maintains high electrical conductivity even as the elastic substrate undergoes extreme deformation. Applying the LM-eKE to human knee joints and fingers, the resistance change during physical activities is under 1.7%, thereby allowing for stable electrical operation of wearable health monitoring devices for tracking electroencephalogram (EEG) signals and other physiological activity.     

Well‐Ordered and High Density Coordination‐Type Bonding to Strengthen Contact of Silver Nanowires on Highly Stretchable Polydimethylsiloxane

Recently, Ag nanowires (AgNWs) has had a great interest as a conducting material for flexible and transparent devices, but it still shows several problems such as the ultimate detachment of AgNWs from substrate and a high contact resistance on AgNW junctions. Therefore, the novel concept to enhance permanent and closed attachment of AgNWs by silane modification to polydimethylsilaoxane (PDMS) substrate well known as high stretchable film with extremly low adhesive is suggested. According to this experiment, higher sigma (σ)‐donating ability and hydrophilicity indicate better electrical and mechanical properties in real device. Especially, densely amine self‐assembled PDMS surface exhibits the strongest contact force to the AgNWs, especially for junction side, and the longest maintenance of hydrophilicity by coordination‐type bonding. In addition, AgNWs adhere permanently to stretchable substrates while simultaneously maintaining high transparency (87%) and high conductivity (27 Ω sq^–1). Consequently, the resulting AgNW film shows excellent mechanical durability which includes enhanced performance of both flexibility and stretchability.     

A Sensing and Stretchable Polymer-Dispersed Liquid Crystal Device Based on Spiderweb-Inspired Silver Nanowires-Micromesh Transparent Electrode

Polymer-dispersed liquid crystal (PDLC) devices are truly promising optical modulators for information display, smart window as well as intelligent photoelectronic applications due to their fast switching, large optical modulation as well as cost-effectiveness. However, realizing highly soft PDLC devices with sensing function remains a grand challenge because of the intrinsic brittleness of traditional transparent conductive electrodes. Here, inspired by spiderweb configuration, a novel type of silver nanowires (AgNWs) micromesh-based stretchable transparent conductive electrodes (STCEs) is developed to support the realization of soft PDLC device. Benefiting from the embedding design of AgNWs micromesh in polydimethylsiloxane (PDMS), the STCEs can maintain excellent electrical conductivity and transparency even in various extreme conditions such as bending, folding, twisting, stretching as well as multiple chemical corrosion. Further, STCEs with the embedded AgNWs micromesh endow the assembled PDLC device with excellent photoelectrical properties including rapid switching speed (<1 s), large optical modulation (69% at 600 nm), as well as robust mechanical stability (bending over 1000 cycles and stretching to 40%). Moreover, the device displays the pressure sensing function with high sensitivity in response to pressure stimulus. It is conceivable that AgNWs micromesh transparent electrodes will shape the next generation of related soft smart electronics.     

A Highly Stretchable Fiber‐Based Triboelectric Nanogenerator for Self‐Powered Wearable Electronics

The development of flexible and stretchable electronics has attracted intensive attention for their promising applications in next‐generation wearable functional devices. However, these stretchable devices that are made in a conventional planar format have largely hindered their development, especially in highly stretchable conditions. Herein, a novel type of highly stretchable, fiber‐based triboelectric nanogenerator (fiber‐like TENG) for power generation is developed. Owing to the advanced structural designs, including the fiber‐convolving fiber and the stretchable electrodes on elastic silicone rubber fiber, the fiber‐like TENG can be operated at stretching mode with high strains up to 70% and is demonstrated for a broad range of applications such as powering a commercial capacitor, LCD screen, digital watch/calculator, and self‐powered acceleration sensor. This work verifies the promising potential of a novel fiber‐based structure for both power generation and self‐powered sensing.     

Gallium-Based Liquid–Solid Biphasic Conductors for Soft Electronics

Soft and stretchable electronics have diverse applications in the fields of compliant bioelectronics, textile-integrated wearables, novel forms of mechanical sensors, electronics skins, and soft robotics. In recent years, multiple material architectures have been proposed for highly deformable circuits that can undergo large tensile strains without losing electronic functionality. Among them, gallium-based liquid metals benefit from fluidic deformability, high electrical conductivity, and self-healing property. However, their deposition and patterning is challenging. Biphasic material architectures are recently proposed as a method to address this problem, by combining advantages of solid-phase materials and composites, with liquid deformability and self-healing of liquid phase conductors, thus moving toward scalable fabrication of reliable stretchable circuits. This article reviews recent biphasic conductor architectures that combine gallium-based liquid-phase conductors, with solid-phase particles and polymers, and their application in fabrication of soft electronic systems. In particular, various material combinations for the solid and liquid phases in the biphasic conductor, as well as methods used to print and pattern biphasic conductive compounds, are discussed. Finally, some applications that benefit from biphasic architectures are reviewed.     

Highly Stretchable and Wearable Thermotherapy Pad with Micropatterned Thermochromic Display Based on Ag Nanowire–Single‐Walled Carbon Nanotube Composite

Due to the increasing interest in wearable devices, flexible and stretchable film heaters have been widely studied, as alternatives to heaters with conventional rigid shapes. Herein, a highly stretchable film heater (SFH) based on the silver nanowire (Ag NW)–single‐walled carbon nanotube composite with a thermochromic display on a polydimethylsiloxane (PDMS) substrate is successfully fabricated. The SFH shows excellent electrical conductivity, high mechanical stretchability, and outstanding reliability, with no significant degradation after 10 000 stretching cycles under tensile strain. The SFH can be heated to the target temperature (≈60 °C) within 30 s at a low applied voltage. In addition, a thermochromic display is fabricated to help prevent the risk of low‐temperature burns. Red (R), green (G), and blue (B) thermochromic microparticles (TMPs) are synthesized using drop‐based microfluidic technology. The TMPs show RGB colors at room temperature but change to a white color above a certain temperature. The TMPs are arrayed into a PDMS stencil on the basis of their particle sizes using the rubbing technique. The micropatterned thermochromic display, which functions as a visual alarm, combined with the SFH can pave the way for the development of thermotherapy pads for next‐generation wearable devices in the medical field.     

Novel Sulfur-Containing Carbon Nanotubes with Graphene Nanoflaps for Stretchable Sensing,Joule Heating,and Electro-Thermal Actuating

Stretchable conductors based on nanopercolation networks have garnered great attention for versatile applications. Carbon nanotubes (CNTs) are well-suited for creating high-efficiency nanopercolation networks. However, the weak interfacial shear strength (IFSS) between CNTs and elastomer hardly dissipates the deformation energy and thus deteriorates the conductive network. Herein, a novel sulfur-containing CNTs attached with abundant graphene nanoflaps using a two-step sulfidation strategy are developed. The sulfur functionality creates a strong interfacial interaction with the elastomer polymer, while the graphene nanoflaps provide an enhanced, intertwined shear interface with elastomer that is capable of efficiently dissipating the deformation energy. As a result, the optimized nanocomposite significantly improves the IFSS between nanofiller and elastomer, displaying remarkable conductive robustness (ΔR/R₀≈1.8 under 200%), superior stretchability (> 450%), and excellent mechanical durability (≈30 000 cycles). Moreover, the nanocomposite demonstrates excellent Joule heating efficiency (≈150 °C in 12 V), stretchable heating conversion (≈200%), and long-term stability (> 24 h). To illustrate its capabilities, the nanocomposite is used to track human physiological signals and perform electric-thermal actuating as a set of soft tongs. It is believed that this innovative approach will provide value for the development of wearable/stretchable devices, as well as human-machine interaction, and bio-robotics in the future.     

Stretchable Energy‐Harvesting Tactile Interactive Interface with Liquid‐Metal‐Nanoparticle‐Based Electrodes

Energy‐harvesting electronic skin (E‐skin) is highly promising for sustainable and self‐powered interactive systems, wearable human health monitors, and intelligent robotics. Flexible/stretchable electrodes and robust energy‐harvesting components are critical in constructing soft, wearable, and energy‐autonomous E‐skin systems. A stretchable energy‐harvesting tactile interactive interface is demonstrated using liquid metal nanoparticles (LM‐NPs)‐based electrodes. This stretchable energy‐harvesting tactile interface relies on triboelectric nanogenerator composed of a galinstan LM‐NP‐based stretchable electrode and patterned elastic polymer friction and encapsulation layer. It provides stable and high open‐circuit voltage (268 V), short‐circuit current (12.06 µA), and transferred charges (103.59 nC), which are sufficient to drive commercial portable electronics. As a self‐powered tactile sensor, it presents satisfactory and repeatable sensitivity of 2.52 V·kPa^?1 and is capable of working as a touch interactive keyboard. The demonstrated stretchable and robust energy‐harvesting E‐skin using LM‐NP‐based electrodes is of great significance in sustainable human–machine interactive system, intelligent robotic skin, security tactile switches, etc.     

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.