Emerging Soft Conductors for Bioelectronic Interfaces

Bidirectional interfacing between electrodes and biological systems has enabled diagnostics and therapeutics in modern medicine; however, the inherent dissimilarity between the soft, ion‐rich, dynamic biological tissues and the rigid, dry, static electronic systems hinders the establishment of effective and reliable bioelectronic interfaces. In the past decade, the scope of flexible/stretchable electronics has been broadened into bioelectronics owing to the need of implementation of various biocompatible soft conductors. Herein, the basic requirements for the construction of both epidermal and implantable bioelectronic interfaces utilizing soft materials are discussed, the most recent progress in the development of soft conductors, which are customized to interface with skin and other tissues, are summarized. An outlook into the remaining obstacles is provided and possible strategies to facilitate technological advances in bioelectronics are also outlined.     

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.     

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.     

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.     

Facile and Rapid Method for Fabricating Liquid Metal Electrodes with Highly Precise Patterns via One‐Step Coating

Gallium‐based alloys, which are virtually non‐toxic liquid metals at room temperature, are considered highly promising electrode materials for state‐of‐the‐art electronics with new form factors. Herein, a facile and rapid method to fabricate liquid metal electrodes with highly precise patterns via a one‐step coating is presented. For this work, polymeric stencil masks with dual structures, comprising upper and lower structures for injecting and molding the liquid metal, respectively, are used for direct patterning of the liquid metal via spray deposition for few seconds, enabling the formation of complex and minute patterns including long thin lines and hollow forms. This method can be adapted to 3D substrates of various materials without any surface treatment, owing to the intrinsic adhesive and flexible properties of the polymeric masks ensuring conformal contact with non‐flat surfaces, and is also expected to be applicable to sub‐micron patterns. In addition, a number of highly flexible/stretchable electronic applications, exhibiting no change in electrical conductivity upon consecutive structural deformations, are demonstrated on various substrates including human skin. It is anticipated that these results will not only spur the further development of flexible/stretchable electronics, but also significantly contribute to the innovative on‐site fabrication of wearable electronics with high durability.     

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.     

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.     

Bio‐Inspired Stretchable,Adhesive, and Conductive Structural Color Film for Visually Flexible Electronics

The rapid progress in flexible electronic devices has attracted immense interest in many applications, such as health monitoring devices, sensory skins, and implantable apparatus. Here, inspired by the adhesion features of mussels and the color shift mechanism of chameleons, a novel stretchable, adhesive, and conductive structural color film is presented for visually flexible electronics. The film is generated by adding a conductive carbon nanotubes polydopamine (PDA) filler into an elastic polyurethane (PU) inverse opal scaffold. Owing to the brilliant flexibility and inverse opal structure of the PU layer, the film shows stable stretchability and brilliant structural color. Besides, the catechol groups on PDA impart the film with high tissue adhesiveness and self‐healing capability. Notably, because of its responsiveness, the resultant film is endowed with color‐changing ability that responds to motions, which can function as dual‐signal soft human‐motion sensors for real‐time color‐sensing and electrical signal monitoring. These features make the bio‐inspired hydrogel‐based electronics highly potential in the flexible electronics field.     

Tuning the Rigidity of Silk Fibroin for the Transfer of Highly Stretchable Electronics

The transfer of stretchable electrodes or devices from one substrate to another thin elastomer is challenging as the elastic stamp often yields a huge strain beyond the stretchability limit of the electrodes at the debonded interface. This will not happen if the stamp is rigid. However, a rigid material cannot be used as the substrate for stretchable electrodes. Herein, silk fibroin with tunable rigidity (Young's modulus can be changed from 134 kPa to 1.84 GPa by controlling the relative humidity) is used to transfer highly stretchable metal networks as highly conformable epidermal electrodes. The silk fibroin stamp is tuned to be rigid during peeling, and then be soft and highly stretchable as a substrate when laminated on moisturized human skin. In addition, the epidermal electrodes exhibit no skin irritation or inflammation after attaching for over 10 d. The high compliance results in a lower interface impedance and lower noises of the electrode in measuring electromyographic signals, compared with commercial Ag‐AgCl gel electrodes. The strategy of tuning the rigidity at different stages of transfer is a general method that can be extended to the transfer of other stretchable electrodes and devices for epidermal electronics, human machine interfaces, and soft robotics.     

Wearable and Implantable Devices for Cardiovascular Healthcare: from Monitoring to Therapy Based on Flexible and Stretchable Electronics

Cardiovascular disease is the leading cause of death and has dramatically increased in recent years. Continuous cardiac monitoring is particularly important for early diagnosis and prevention, and flexible and stretchable electronic devices have emerged as effective tools for this purpose. Their thin, soft, and deformable features allow intimate and long‐term integration with biotissues, which enables continuous, high‐fidelity, and sometimes large‐area cardiac monitoring on the skin and/or heart surface. In addition to monitoring, intimate contact is also crucial for high‐precision therapies. Combined with tissue engineering, soft bioelectronics have also demonstrated the capability to repair damaged cardiac tissues. This review highlights the recent advances in wearable and implantable devices based on flexible and stretchable electronics for cardiovascular monitoring and therapy. First, wearable/implantable soft bioelectronics for cardiovascular monitoring (e.g., the electrocardiogram, blood pressure, and oxygen saturation level) are reviewed. Then, advances in cardiovascular therapy based on soft bioelectronics (e.g., mesh pacing, ablation, robotic sleeves, and electronic stents) are discussed. Finally, device‐assisted tissue engineering therapy (e.g., functional electronic scaffolds and in vitro cardiac platforms) is discussed.     

Design and implementation of flexible and stretchable systems

This paper presents a summary of the modeling and technology developments for flexible and stretchable electronics. These technologies can achieve mechanically bendable and stretchable subsystems by incorporating the electronic circuit into a matrix made of a soft polymer. The base substrate used for the fabrication of flexible circuits is a uniform polyimide layer, while silicones or polyurethanes materials are preferred for the stretchable circuits. The method developed for chip embedding and interconnections is named Ultra Thin Chip Package (UTCP). Extensions of this technology can be achieved by stacking and embedding thin dies in polyimide, providing large benefits in electrical performance and still allowing some mechanical flexibility. These flexible circuits can be converted into stretchable circuits by replacing the polyimide by a soft and elastic silicone material.The integration of ultra thin dies at package level, with thickness in the range of 10-30 μm, into flexible and/or stretchable materials are demonstrated. Furthermore, the design and reliability test of stretchable metal interconnections at board level are analyzed by both experiments and finite element modeling. We have shown through finite element modeling and experimental validation that an appropriate thermo-mechanical design is necessary to achieve mechanically reliable circuits and thermally optimized packages.     

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.     

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.     

All‐Printed Flexible and Stretchable Electronics with Pressing or Freezing Activatable Liquid‐Metal–Silicone Inks

Liquid‐metal (LM)‐based flexible and stretchable electronics have attracted widespread interest in wearable computing, human–machine interaction, and soft robotics. However, many current examples are one‐off prototypes, whereas future implementation requires mass production. To address this critical challenge, an integrated multimaterial 3D printing process composed of direct ink writing (DIW) of sealing silicone elastomer and special LM‐silicone (LMS) inks for manufacturing high‐performance LM‐based flexible and stretchable electronics is presented. The LMS ink is a concentrated mixture of LM microdroplets and silicone elastomer and exhibits excellent printability for DIW printing. Guided by a verified theoretical model, a printing process with high resolution and high speed can be easily implemented. Although LMS is not initially conductive, it can be activated by pressing or freezing. Activated LMS possesses good conductivity and significant electrical response to strain. Owing to LMS's unique structure, LMS‐embedded flexible electronics exhibit great damage mitigation, in that no leaking occurs even when damaged. To demonstrate the flexibility of this process in fabricating LM‐based flexible electronics, multilayer soft circuits, strain sensors, and data gloves are printed and investigated. Notably, utilizing LMS's unique activating property, some functional circuits such as one‐time pressing/freezing‐on switch can be printed without any structural design.     

Structure Design and Performance of Hybridized Nanogenerators

Intelligent energy generation from ambient environment by various nanogenerators is desirable to realize self‐powered operation of electronics. By integrating two or more kinds of nanogenerators, a hybridized nanogenerator provides a possible solution to largely increase the total electric power, and thus has been considered as one of the most significant energy‐related technologies. Here, emerging advancements in hybridized nanogenerators are summarized in terms of their structures, principles, and potential applications. In particular, one‐structure‐based coupled nanogenerators based on multifunctional energy‐scavenging materials and the interface regulation of solar cells by inner nanogenerators are discussed. For potential applications in wearable electronics, the new progress on flexible hybridized nanogenerators is presented on the basis of stretchable and mechanically durable materials, substrates, and electrodes. With the advances highlighted here and the ongoing research efforts, the continuous breakthrough in hybridized nanogenerators for multiple energy scavenging and their extensive applications is foreseeable in the future.     

Metal/Polymer Based Stretchable Antenna for Constant Frequency Far‐Field Communication in Wearable Electronics

Body integrated wearable electronics can be used for advanced health monitoring, security, and wellness. Due to the complex, asymmetric surface of human body and atypical motion such as stretching in elbow, finger joints, wrist, knee, ankle, etc. electronics integrated to body need to be physically flexible, conforming, and stretchable. In that context, state‐of‐the‐art electronics are unusable due to their bulky, rigid, and brittle framework. Therefore, it is critical to develop stretchable electronics which can physically stretch to absorb the strain associated with body movements. While research in stretchable electronics has started to gain momentum, a stretchable antenna which can perform far‐field communications and can operate at constant frequency, such that physical shape modulation will not compromise its functionality, is yet to be realized. Here, a stretchable antenna is shown, using a low‐cost metal (copper) on flexible polymeric platform, which functions at constant frequency of 2.45 GHz, for far‐field applications. While mounted on a stretchable fabric worn by a human subject, the fabricated antenna communicated at a distance of 80 m with 1.25 mW transmitted power. This work shows an integration strategy from compact antenna design to its practical experimentation for enhanced data communication capability in future generation wearable electronics.     

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.     

Emerging Design Strategies Toward Developing Next-Generation Implantable Batteries and Supercapacitors

In recent years, the development of implantable bioelectronics has garnered significant attention. With the continuous advancement of IoT and information technology, implantable bioelectronics can be utilized more effectively for health monitoring to enhance treatment outcomes, reduce healthcare costs, and improve quality of life. Implantable energy storage devices have been widely studied as critical components for energy supply. Conventional power sources are bulky, inflexible, and potentially contain materials that are dangerous to the body. Meanwhile, human tissues are soft, flexible, dynamic, and closed, which puts new requirements on energy storage devices to improve the safety, stability, and matching of implantable batteries or supercapacitors. Herein, recent advances in state-of-the-art nonconventional power options for implantable electronics, specifically biocompatible, miniaturized, stretchable/deformable, biodegradable/bioresorbable, edible, and injectable energy storage devices, are reviewed in this paper. The material strategy and architectural design of the next-generation implantable energy storage device are discussed, including the selection principle of electrolytes, the all-in-one structure design strategy, and the way to realize self-charging. Finally, the challenges and prospects of emerging design strategies toward developing next-generation implantable batteries and supercapacitors for the future are put forward.     

Stretchable,Skin‐Mountable,and Wearable Strain Sensors and Their Potential Applications: A Review

There is a growing demand for flexible and soft electronic devices. In particular, stretchable, skin‐mountable, and wearable strain sensors are needed for several potential applications including personalized health‐monitoring, human motion detection, human‐machine interfaces, soft robotics, and so forth. This Feature Article presents recent advancements in the development of flexible and stretchable strain sensors. The article shows that highly stretchable strain sensors are successfully being developed by new mechanisms such as disconnection between overlapped nanomaterials, crack propagation in thin films, and tunneling effect, different from traditional strain sensing mechanisms. Strain sensing performances of recently reported strain sensors are comprehensively studied and discussed, showing that appropriate choice of composite structures as well as suitable interaction between functional nanomaterials and polymers are essential for the high performance strain sensing. Next, simulation results of piezoresistivity of stretchable strain sensors by computational models are reported. Finally, potential applications of flexible strain sensors are described. This survey reveals that flexible, skin‐mountable, and wearable strain sensors have potential in diverse applications while several grand challenges have to be still overcome.