Recent Advances in 1D Stretchable Electrodes and Devices for Textile and Wearable Electronics: Materials,Fabrications, and Applications

Research on wearable electronic devices that can be directly integrated into daily textiles or clothes has been explosively grown holding great potential for various practical wearable applications. These wearable electronic devices strongly demand 1D electronic devices that are light–weight, weavable, highly flexible, stretchable, and adaptable to comport to frequent deformations during usage in daily life. To this end, the development of 1D electrodes with high stretchability and electrical performance is fundamentally essential. Herein, the recent process of 1D stretchable electrodes for wearable and textile electronics is described, focusing on representative conductive materials, fabrication techniques for 1D stretchable electrodes with high performance, and designs and applications of various 1D stretchable electronic devices. To conclude, discussions are presented regarding limitations and perspectives of current materials and devices in terms of performance and scientific understanding that should be considered for further advances.     

Wearable Electronics Based on Stretchable Organic Semiconductors

Wearable electronics are attracting increasing interest due to the emerging Internet of Things (IoT). Compared to their inorganic counterparts, stretchable organic semiconductors (SOSs) are promising candidates for wearable electronics due to their excellent properties, including light weight, stretchability, dissolubility, compatibility with flexible substrates, easy tuning of electrical properties, low cost, and low temperature solution processability for large-area printing. Considerable efforts have been dedicated to the fabrication of SOS-based wearable electronics and their potential applications in various areas, including chemical sensors, organic light emitting diodes (OLEDs), organic photodiodes (OPDs), and organic photovoltaics (OPVs), have been demonstrated. In this review, some recent advances of SOS-based wearable electronics based on the classification by device functionality and potential applications are presented. In addition, a conclusion and potential challenges for further development of SOS-based wearable electronics are also discussed.     

Plasticizing Silk Protein for On‐Skin Stretchable Electrodes

Soft and stretchable electronic devices are important in wearable and implantable applications because of the high skin conformability. Due to the natural biocompatibility and biodegradability, silk protein is one of the ideal platforms for wearable electronic devices. However, the realization of skin‐conformable electronic devices based on silk has been limited by the mechanical mismatch with skin, and the difficulty in integrating stretchable electronics. Here, silk protein is used as the substrate for soft and stretchable on‐skin electronics. The original high Young's modulus (5–12 GPa) and low stretchability (<20%) are tuned into 0.1–2 MPa and > 400%, respectively. This plasticization is realized by the addition of CaCl₂ and ambient hydration, whose mechanism is further investigated by molecular dynamics simulations. Moreover, highly stretchable (>100%) electrodes are obtained by the thin‐film metallization and the formation of wrinkled structures after ambient hydration. Finally, the plasticized silk electrodes, with the high electrical performance and skin conformability, achieve on‐skin electrophysiological recording comparable to that by commercial gel electrodes. The proposed skin‐conformable electronics based on biomaterials will pave the way for the harmonized integration of electronics into human.     

基于导电纤维的柔性电子器件研究进展

柔性电子器件具有优异的灵活性,实现了与服装的无缝集成,在各种实际的可穿戴应用中具有巨大的潜力。一维纤维状电子器件由于其优异的柔韧性、可编织性及舒适性成为智能可穿戴领域的研究热点。首先,综述了用于纤维状柔性电子器件的一维可拉伸电极的研究进展,然后详细介绍了高性能一维纤维状柔性电子器件制备过程中具有代表性的导电材料、制造技术及一维柔性纤维进一步应用于各类电子器件的主要制备方法,另外总结了近年来基于柔性纤维状电子器件在智能可穿戴领域的应用。最后对一维纤维基智能可穿戴电子器件的机遇和挑战进行了批判性思考。      

Self-healing flexible/stretchable energy storage devices

During the past decade, flexible/stretchable energy storage devices have garnered increasing attention, with the successful development of wearable electronics. However, due to the repeated deformation accompanied with the electrochemical depletion process, these devices suffer from unavoidable damage, including cracks, crazing, puncture and delamination, which can lead to serious performance degradation or even safety issues. Simultaneously, inspired by biological organs, self-healing capability is found to be a promising approach to address these issues by restoring the mechanical and electrochemical performance. This review first summarizes the structural design and features of various flexible/stretchable energy storage devices, from 1D to 3D configurations. Then, basic concepts and three self-healing mechanisms, including capsule-based systems, vascular-based systems, and intrinsic healing systems are analyzed along with a brief look at existing applications. Then we review all the important parts of state-of-art flexible/stretchable self-healing supercapacitors and batteries including electrodes, electrolytes, substrates and encapsulation. Moreover, a detailed evaluation of methodologies for flexibility, stretchability and self-healing capabilities are described in detail. Finally, the critical challenges and prospects of future promising solutions for self-healing flexible/stretchable energy storage devices or even electronics are provided.     

Flexible Hybrid Sensors for Health Monitoring: Materials and Mechanisms to Render Wearability

Wearable electronics have revolutionized the way physiological parameters are sensed, detected, and monitored. In recent years, advances in flexible and stretchable hybrid electronics have created emergent properties that enhance the compliance of devices to our skin. With their unobtrusive attributes, skin conformable sensors enable applications toward real-time disease diagnosis and continuous healthcare monitoring. Herein, critical perspectives of flexible hybrid electronics toward the future of digital health monitoring are provided, emphasizing its role in physiological sensing. In particular, the strategies within the sensor composition to render flexibility and stretchability while maintaining excellent sensing performance are considered. Next, novel approaches to the functionalization of the sensor for physical or biochemical stimuli are extensively covered. Subsequently, wearable sensors measuring physical parameters such as strain, pressure, temperature, as well as biological changes in metabolites and electrolytes are reported. Finally, their implications toward early disease detection and monitoring are discussed, concluding with a future perspective into the challenges and opportunities in emerging wearable sensor designs for the next few years.     

Biofriendly,Stretchable, and Reusable Hydrogel Electronics as Wearable Force Sensors

The ever‐growing overlap between stretchable electronic devices and wearable healthcare applications is igniting the discovery of novel biocompatible and skin‐like materials for human‐friendly stretchable electronics fabrication. Amongst all potential candidates, hydrogels with excellent biocompatibility and mechanical features close to human tissues are constituting a promising troop for realizing healthcare‐oriented electronic functionalities. In this work, based on biocompatible and stretchable hydrogels, a simple paradigm to prototype stretchable electronics with an embedded three‐dimensional (3D) helical conductive layout is proposed. Thanks to the 3D helical structure, the hydrogel electronics present satisfactory mechanical and electrical robustness under stretch. In addition, reusability of stretchable electronics is realized with the proposed scenario benefiting from the swelling property of hydrogel. Although losing water would induce structure shrinkage of the hydrogel network and further undermine the function of hydrogel in various applications, the worn‐out hydrogel electronics can be reused by simply casting it in water. Through such a rehydration procedure, the dehydrated hydrogel can absorb water from the surrounding and then the hydrogel electronics can achieve resilience in mechanical stretchability and electronic functionality. Also, the ability to reflect pressure and strain changes has revealed the hydrogel electronics to be promising for advanced wearable sensing applications.     

Stretchable,Large‐area Organic Electronics

Stretchability will significantly expand the application scope of electronics, particularly large‐area electronics—displays, sensors, and actuators. If arbitrary surfaces and movable parts could be covered with stretchable electronics, which is impossible with conventional electronics, new classes of applications are expected to emerge. A large hurdle is manufacturing electrical wiring with high conductivity, high stretchability, and large‐area compatibility. This Review describes stretchable, large‐area electronics based on organic field‐effect transistors for applications to sensors and displays. First, novel net‐shaped organic transistors are employed to realize stretchable, large‐area sensor networks that detect distributions of pressure and temperature simultaneously. The whole system is functional even when it is stretched by 25%. In order to further improve stretchability, printable elastic conductors are developed by dispersing single‐walled carbon nanotubes (SWNTs) as dopants uniformly in rubbers. Further, we describe integration of printable elastic conductors with organic transistors to construct a rubber‐like stretchable active matrix for large‐area sensor and display applications. Finally, we will discuss the future prospects of stretchable, large‐area electronics with delineating a picture of the next‐generation human/machine interfaces from the aspect of materials science and electronic engineering.     

An All‐Stretchable‐Component Sodium‐Ion Full Battery

Stretchable energy‐storage devices receive considerable attention due to their promising applications in future wearable technologies. However, they currently suffer from many problems, including low utility of active materials, limited multidirectional stretchability, and poor stability under stretched conditions. In addition, most proposed designs use one or more rigid components that fail to meet the stretchability requirement for the entire device. Here, an all‐stretchable‐component sodium‐ion full battery based on graphene‐modified poly(dimethylsiloxane) sponge electrodes and an elastic gel membrane is developed for the first time. The battery exhibits reasonable electrochemical performance and robust mechanical deformability; its electrochemical characteristics can be well‐maintained under many different stretched conditions and after hundreds of stretching–release cycles. This novel design integrating all stretchable components provides a pathway toward the next generation of wearable energy devices in modern electronics.     

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

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

Stretchable Conductive Polymers and Composites Based on PEDOT and PEDOT:PSS

The conductive polymer poly(3,4‐ethylenedioxythiophene) (PEDOT), and especially its complex with poly(styrene sulfonate) (PEDOT:PSS), is perhaps the most well‐known example of an organic conductor. It is highly conductive, largely transmissive to light, processible in water, and highly flexible. Much recent work on this ubiquitous material has been devoted to increasing its deformability beyond flexibility—a characteristic possessed by any material that is sufficiently thin—toward stretchability, a characteristic that requires engineering of the structure at the molecular‐ or nanoscale. Stretchability is the enabling characteristic of a range of applications envisioned for PEDOT in energy and healthcare, such as wearable, implantable, and large‐area electronic devices. High degrees of mechanical deformability allow intimate contact with biological tissues and solution‐processable printing techniques (e.g., roll‐to‐roll printing). PEDOT:PSS, however, is only stretchable up to around 10%. Here, the strategies that have been reported to enhance the stretchability of conductive polymers and composites based on PEDOT and PEDOT:PSS are highlighted. These strategies include blending with plasticizers or polymers, deposition on elastomers, formation of fibers and gels, and the use of intrinsically stretchable scaffolds for the polymerization of PEDOT.     

3D Printed Stretchable Tactile Sensors

The development of methods for the 3D printing of multifunctional devices could impact areas ranging from wearable electronics and energy harvesting devices to smart prosthetics and human–machine interfaces. Recently, the development of stretchable electronic devices has accelerated, concomitant with advances in functional materials and fabrication processes. In particular, novel strategies have been developed to enable the intimate biointegration of wearable electronic devices with human skin in ways that bypass the mechanical and thermal restrictions of traditional microfabrication technologies. Here, a multimaterial, multiscale, and multifunctional 3D printing approach is employed to fabricate 3D tactile sensors under ambient conditions conformally onto freeform surfaces. The customized sensor is demonstrated with the capabilities of detecting and differentiating human movements, including pulse monitoring and finger motions. The custom 3D printing of functional materials and devices opens new routes for the biointegration of various sensors in wearable electronics systems, and toward advanced bionic skin applications.     

Flexible/Stretchable Supercapacitors with Novel Functionality for Wearable Electronics

With the miniaturization of personal wearable electronics, considerable effort has been expended to develop high-performance flexible/stretchable energy storage devices for powering integrated active devices. Supercapacitors can fulfill this role owing to their simple structures, high power density, and cyclic stability. Moreover, a high electrochemical performance can be achieved with flexible/stretchable supercapacitors, whose applications can be expanded through the introduction of additional novel functionalities. Here, recent advances in and future prospects for flexible/stretchable supercapacitors with innate functionalities are covered, including biodegradability, self-healing, shape memory, energy harvesting, and electrochromic and temperature tolerance, which can contribute to reducing e-waste, ensuring device integrity and performance, enabling device self-charging following exposure to surrounding stimuli, displaying the charge status, and maintaining the performance under a wide range of temperatures. Finally, the challenges and perspectives of high-performance all-in-one wearable systems with integrated functional supercapacitors for future practical application are discussed.     

Stretchable Transistor-Structured Artificial Synapses for Neuromorphic Electronics

Stretchable synaptic transistors, a core technology in neuromorphic electronics, have functions and structures similar to biological synapses and can concurrently transmit signals and learn. Stretchable synaptic transistors are usually soft and stretchy and can accommodate various mechanical deformations, which presents significant prospects in soft machines, electronic skin, human–brain interfaces, and wearable electronics. Considerable efforts have been devoted to developing stretchable synaptic transistors to implement electronic device neuromorphic functions, and remarkable advances have been achieved. Here, this review introduces the basic concept of artificial synaptic transistors and summarizes the recent progress in device structures, functional-layer materials, and fabrication processes. Classical stretchable synaptic transistors, including electric double-layer synaptic transistors, electrochemical synaptic transistors, and optoelectronic synaptic transistors, as well as the applications of stretchable synaptic transistors in light-sensory systems, tactile-sensory systems, and multisensory artificial-nerves systems, are discussed. Finally, the current challenges and potential directions of stretchable synaptic transistors are analyzed. This review presents a detailed introduction to the recent progress in stretchable synaptic transistors from basic concept to applications, providing a reference for the development of stretchable synaptic transistors in the future.     

Toward Environmentally Robust Organic Electronics: Approaches and Applications

Recent interest in flexible electronics has led to a paradigm shift in consumer electronics, and the emergent development of stretchable and wearable electronics is opening a new spectrum of ubiquitous applications for electronics. Organic electronic materials, such as π‐conjugated small molecules and polymers, are highly suitable for use in low‐cost wearable electronic devices, and their charge‐carrier mobilities have now exceeded that of amorphous silicon. However, their commercialization is minimal, mainly because of weaknesses in terms of operational stability, long‐term stability under ambient conditions, and chemical stability related to fabrication processes. Recently, however, many attempts have been made to overcome such instabilities of organic electronic materials. Here, an overview is provided of the strategies developed for environmentally robust organic electronics to overcome the detrimental effects of various critical factors such as oxygen, water, chemicals, heat, and light. Additionally, molecular design approaches to π‐conjugated small molecules and polymers that are highly stable under ambient and harsh conditions are explored; such materials will circumvent the need for encapsulation and provide a greater degree of freedom using simple solution‐based device‐fabrication techniques. Applications that are made possible through these strategies are highlighted.     

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.     

Stretchable Thin‐Film Electrodes for Flexible Electronics with High Deformability and Stretchability

Flexible and stretchable electronics represent today's cutting‐edge electronic technologies. As the most‐fundamental component of electronics, the thin‐film electrode remains the research frontier due to its key role in the successful development of flexible and stretchable electronic devices. Stretchability, however, is generally more challenging to achieve than flexibility. Stretchable electronic devices demand, above all else, that the thin‐film electrodes have the capacity to absorb a large level of strain (>>1%) without obvious changes in their electrical performance. This article reviews the progress in strategies for obtaining highly stretchable thin‐film electrodes. Applications of stretchable thin‐film electrodes fabricated via these strategies are described. Some perspectives and challenges in this field are also put forward.     

Organic Photodetectors for Next-Generation Wearable Electronics

Next-generation wearable electronics will need to be mechanically flexible and stretchable such that they can be conformally attached onto the human body. Photodetectors that are available in today's market are based on rigid inorganic crystalline materials and they have limited mechanical flexibility. In contrast, photodetectors based on organic polymers and molecules have emerged as promising alternatives due to their inherent mechanical softness, ease of processing, tunable optoelectronic properties, good light sensing performance, and biocompatibility. Here, the recent advances of organic photodetectors in terms of both optoelectronic and mechanical properties are outlined and discussed, and their application in wearable electronics including health monitoring sensors, artificial vision, and self-powering integrated devices are highlighted.     

Mechanics of stretchable electronics

Recent advances in mechanics and materials provide routes to develop stretchable electronics that offer performance of conventional wafer-based devices but with the ability to be deformed to arbitrary shape. Many new applications become possible ranging from electronic eye cameras to wearable electronics, to bio-integrated therapeutic devices. This paper reviews mechanics of stretchable electronics in terms of two main forms of stretchable designs. One is wavy design, which can provide one-dimensional stretchability. The other is island-bridge design, which can be stretched in all directions. Mechanics models and their comparisons to experiments and finite element simulations are reviewed for these two designs. The results provide design guidelines for the development of stretchable electronics.