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.     

Cucurbit[n]uril Supramolecular Hydrogel Networks as Tough and Healable Adhesives

Supramolecular noncovalent interactions are widely found in natural adhesion phenomena to control macroscopic adhesion and accomplish a variety of complex functions. Such supramolecular adhesives could impart the interfaces with intriguing properties, e.g., energy dissipation and self‐healing, on account of their dynamic nature. Here, we demonstrate that cucurbit[8]uril (CB[8])‐based supramolecular hydrogel networks can function as dynamic adhesives for diverse nonporous (e.g., glass, stainless steel, aluminum, copper, and titanium) and porous substrates (wood and bone). Without any surface prefunctionalization or introduction of curing agents, these CB[8] hydrogel networks can be readily applied by curing around the softening temperature, forming a tough and healable adhesive interlayer. The ability to fabricate a robust sandwich model consisting of substrate–CB[8] hydrogel network–substrate enables a number of applications including stretchable and wearable electronics, hybrid systems for biomedical devices or tissue/bone regeneration.     

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.     

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.     

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.     

A High‐Capacitance Salt‐Free Dielectric for Self‐Healable,Printable, and Flexible Organic Field Effect Transistors and Chemical Sensor

Printable and flexible electronics attract sustained attention for their low cost, easy scale up, and potential application in wearable and implantable sensors. However, they are susceptible to scratching, rupture, or other damage from bending or stretching due to their “soft” nature compared to their rigid counterparts (Si‐based electronics), leading to loss of functionality. Self‐healing capability is highly desirable for these “soft” electronic devices. Here, a versatile self‐healing polymer blend dielectric is developed with no added salts and it is integrated into organic field transistors (OFETs) as a gate insulator material. This polymer blend exhibits an unusually high thin film capacitance (1400 nF cm^?2 at 120 nm thickness and 20–100 Hz). Furthermore, it shows pronounced electrical and mechanical self‐healing behavior, can serve as the gate dielectric for organic semiconductors, and can even induce healing of the conductivity of a layer coated above it together with the process of healing itself. Based on these attractive properties, we developed a self‐healable, low‐voltage operable, printed, and flexible OFET for the first time, showing promise for vapor sensing as well as conventional OFET applications.     

Stretchable and Transparent Biointerface Using Cell‐Sheet–Graphene Hybrid for Electrophysiology and Therapy of Skeletal Muscle

Implantable electronic devices for recording electrophysiological signals and for stimulating muscles and nerves have been widely used throughout clinical medicine. Mechanical mismatch between conventional rigid biomedical devices and soft curvilinear tissues, however, has frequently resulted in a low signal to noise ratio and/or mechanical fatigue and scarring. Multifunctionality ranging from various sensing modalities to therapeutic functions is another important goal for implantable biomedical devices. Here, a stretchable and transparent medical device using a cell‐sheet–graphene hybrid is reported, which can be implanted to form a high quality biotic/abiotic interface. The hybrid is composed of a sheet of C2C12 myoblasts on buckled, mesh‐patterned graphene electrodes. The graphene electrodes monitor and actuate the C2C12 myoblasts in vitro, serving as a smart cell culture substrate that controls their aligned proliferation and differentiation. This stretchable and transparent cell‐sheet–graphene hybrid can be transplanted onto the target muscle tissue, to record electromyographical signals, and stimulate implanted sites electrically and/or optically in vivo. Additional cellular therapeutic effect of the cell‐sheet–graphene hybrid is obtained by integrated myobalst cell sheets. Any immune responses within implanted muscle tissues are not observed. This multifunctional device provides many new opportunities in the emerging field of soft bioelectronics.     

Bioinspired Self-healing Soft Electronics

Inspired by nature, various self-healing materials that can recover their physical properties after external damage have been developed. Recently, self-healing materials have been widely used in electronic devices for improving durability and protecting the devices from failure during operation. Moreover, self-healing materials can integrate many other intriguing properties of biological systems, such as stretchability, mechanical toughness, adhesion, and structural coloration, providing additional fascinating experiences. All of these inspirations have attracted extensive research on bioinspired self-healing soft electronics. This review presents a detailed discussion on bioinspired self-healing soft electronics. Firstly, two main healing mechanisms are introduced. Then, four categories of self-healing materials in soft electronics, including insulators, semiconductors, electronic conductors, and ionic conductors, are reviewed, and their functions, working principles, and applications are summarized. Finally, human-inspired self-healing materials and animal-inspired self-healing materials as well as their applications, such as organic field-effect transistors (OFETs), pressure sensors, strain sensors, chemical sensors, triboelectric nanogenerators (TENGs), and soft actuators, are introduced. This cutting-edge and promising field is believed to stimulate more excellent cross-discipline works in material science, flexible electronics, and novel sensors, accelerating the development of applications in human motion monitoring, environmental sensing, information transmission, etc.     

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.     

Wearable and Implantable Triboelectric Nanogenerators

Triboelectric nanogenerators (TENGs) are a promising technology to convert mechanical energy to electrical energy based on coupled triboelectrification and electrostatic induction. With the rapid development of functional materials and manufacturing techniques, wearable and implantable TENGs have evolved into playing important roles in clinic and daily life from in vitro to in vivo. These flexible and light membrane‐like devices have the potential to be a new power supply or sensor element, to meet the special requirements for portable electronics, promoting innovation in electronic devices. In this review, the recent advances in wearable and implantable TENGs as sustainable power sources or self‐powered sensors are reviewed. In addition, the remaining challenges and future possible improvements of wearable and implantable TENG‐based self‐powered systems are discussed.     

High density interconnects and flexible hybrid assemblies foractive biomedical implants

Advanced microtechnologies offer new opportunities for the development of active implants that go beyond the design of pacemakers and cochlea implants. Examples of future implants include neural and muscular stimulators, implantable drug delivery systems, intracorporal monitoring devices and body fluid control systems. The active microimplants demand a high degree of device miniaturization without compromising on design flexibility and biocompatibility requirements. With the need for integrating various microcomponents for a complex retina stimulator device, we have developed a novel technique for microassembly and high-density interconnects employing flexible, ultra-thin polymer based substrates. Pads for interconnections, conductive lines, and microelectrodes were embedded into the polyimide substrate as thin films. Photolithography and sputtering has been employed to pattern the microstructures. The novel “MicroFlex interconnection (MFI)” technology was developed to achieve chip size package (CSP) dimensions without the requirement of using bumped flip chips (FC). The MFI is based on a rivet like approach that yields an electrical and mechanical contact between the pads on the flexible polyimide substrate and the bare chips or electronic components. Center to center bond pad distances smaller than 100 μm were accomplished. The ultra thin substrates and the MFI technology was proven to be biocompatible. Electrical and mechanical tests confirmed that interconnects and assembly of bare chips are reliable and durable. Based on our experience with the retina stimulator implant, we defined design rules regarding the flexible substrate, the bond pads, and the embedded conductive tracks. It is concluded that the MFI opens new venues for a novel generation of active implants with advanced sensing, actuation, and signal processing properties     

Flexible Hybrid Electronics: Direct Interfacing of Soft and Hard Electronics for Wearable Health Monitoring

The interfacing of soft and hard electronics is a key challenge for flexible hybrid electronics. Currently, a multisubstrate approach is employed, where soft and hard devices are fabricated or assembled on separate substrates, and bonded or interfaced using connectors; this hinders the flexibility of the device and is prone to interconnect issues. Here, a single substrate interfacing approach is reported, where soft devices, i.e., sensors, are directly printed on Kapton polyimide substrates that are widely used for fabricating flexible printed circuit boards (FPCBs). Utilizing a process flow compatible with the FPCB assembly process, a wearable sensor patch is fabricated composed of inkjet‐printed gold electrocardiography (ECG) electrodes and a stencil‐printed nickel oxide thermistor. The ECG electrodes provide 1 mVp–p ECG signal at 4.7 cm electrode spacing and the thermistor is highly sensitive at normal body temperatures, and demonstrates temperature coefficient, α ≈ –5.84% K^–1 and material constant, β ≈ 4330 K. This sensor platform can be extended to a more sophisticated multisensor platform where sensors fabricated using solution processable functional inks can be interfaced to hard electronics for health and performance monitoring, as well as internet of things applications.     

An Autofluorescent Hydrogel with Water-Dependent Emission for Dehydration-Visualizable Smart Wearable Electronics

Wearable flexible electronics that are derived from hydrogels inevitably undergo dehydration, and the sensing performance is highly affected because the stretchability and conductivity weaken. Monitoring the water retention rate of hydrogels as they operate without dismantling the assembled sensing device is vital for evaluating sensing performances and intervening in a timely manner to address the problem. However, relevant research is still lacking. Herein, an autofluorescent hydrogel is engineered based on clusterization-triggered emission (CTE) for wearable strain-sensing electronics that can undergo self-visualizing dehydration. The fluorescence intensity of the CTE-type autofluorescent hydrogel depends on the aggregation level of molecule clusters that are dangled on the gel networks, which is dominated by the water retention rate of the hydrogel. Thus, the dehydration process can be reflected by the fluorescent images taken in a scenario of long-term strain-sensing. This strategy helps the operator evaluate the water retention rate of the hydrogel without removing it from the assembled electronics and then quickly address the problem. In addition, this strategy is also applicable for dehydration-tolerant systems, demonstrating the versatility of the autofluorescent hydrogel. Overall, the CTE-type autofluorescent hydrogel will promote the development of high-performance and smart wearable electronics.     

3D Printing of Multifunctional Hydrogels

3D printing technology has been widely explored for the rapid design and fabrication of hydrogels, as required by complicated soft structures and devices. Here, a new 3D printing method is presented based on the rheology modifier of Carbomer for direct ink writing of various functional hydrogels. Carbomer is shown to be highly efficient in providing ideal rheological behaviors for multifunctional hydrogel inks, including double network hydrogels, magnetic hydrogels, temperature‐sensitive hydrogels, and biogels, with a low dosage (at least 0.5% w/v) recorded. Besides the excellent printing performance, mechanical behaviors, and biocompatibility, the 3D printed multifunctional hydrogels enable various soft devices, including loadable webs, soft robots, 4D printed leaves, and hydrogel Petri dishes. Moreover, with its unprecedented capability, the Carbomer‐based 3D printing method opens new avenues for bioprinting manufacturing and integrated hydrogel devices.     

A Skin‐Inspired Substrate with Spaghetti‐Like Multi‐Nanofiber Network of Stiff and Elastic Components for Stretchable Electronics

Mimicking the skin's non‐linear self‐limiting mechanical characteristics is of great interest. Skin is soft at low strain but becomes stiff at high strain and thereby can protect human tissues and organs from high mechanical loads. Herein, the design of a skin‐inspired substrate is reported based on a spaghetti‐like multi‐nanofiber network (SMNN) of elastic polyurethane (PU) nanofibers (NFs) sandwiched between stiff poly(vinyldenefluoride‐co‐trifluoroethylene) (P(VDF‐TrFE)) NFs layers embedded in polydimethylsiloxane elastomer. The elastic moduli of the stretchable skin‐inspired substrate can be tuned in a range that matches well with the mechanical properties of skins by adjusting the loading ratios of the two NFs. Confocal imaging under stretching indicates that PU NFs help maintain the stretchability while adding stiff P(VDF‐TrFE) NFs to control the self‐limiting characteristics. Interestingly, the Au layer on the substrate indicates a negligible change in the resistance under cyclic (up to 7000 cycles at 35% strain) and dynamic stretching (up to 35% strain), which indicates the effective absorption of stress by the SMNN. A stretchable chemoresistive gas sensor on the skin‐inspired substrate also demonstrates a reasonable stability in NO₂ sensing response under strain up to 30%. The skin‐inspired substrate with SMNN provides a step toward ultrathin stretchable electronics.     

Chemical Sensing Systems that Utilize Soft Electronics on Thin Elastomeric Substrates with Open Cellular Designs

A collection of materials and device architectures are introduced for thin, stretchable arrays of ion sensors that mount on open cellular substrates to facilitate solution exchange for use in biointegrated electronics. The results include integration strategies and studies of fundamental characteristics in chemical sensing and mechanical response. The latter involves experimental measurements and theoretical simulations that establish important considerations in the design of low modulus, stretchable properties in cellular substrates, and in the realization of advanced capabilities in spatiotemporal mapping of chemicals' gradients. As the chemical composition of extracellular fluids contains valuable information related to biological function, the concepts introduced here have potential utility across a range of skin‐ and internal‐organ‐integrated electronics where soft mechanics, fluidic permeability, and advanced chemical sensing capabilities are key requirements.     

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.     

Powering Implantable and Ingestible Electronics

Implantable and ingestible biomedical electronic devices can be useful tools for detecting physiological and pathophysiological signals, and providing treatments that cannot be done externally. However, one major challenge in the development of these devices is the limited lifetime of their power sources. The state-of-the-art of powering technologies for implantable and ingestible electronics is reviewed here. The structure and power requirements of implantable and ingestible biomedical electronics are described to guide the development of powering technologies. These powering technologies include novel batteries that can be used as both power sources and for energy storage, devices that can harvest energy from the human body, and devices that can receive and operate with energy transferred from exogenous sources. Furthermore, potential sources of mechanical, chemical, and electromagnetic energy present around common target locations of implantable and ingestible electronics are thoroughly analyzed; energy harvesting and transfer methods befitting each energy source are also discussed. Developing power sources that are safe, compact, and have high volumetric energy densities is essential for realizing long-term in-body biomedical electronics and for enabling a new era of personalized healthcare.     

A Universal Size Design Principle for Stretchable Inorganic Electronics to Work Consistently under Different Interface Conditions

Stretchable inorganic electronics are usually designed and calibrated under free interface condition, while the interface conditions between the devices and skins/organs in practical applications are rather complex (free, slidable, or bonded) and may switch among them. In the ideal situation, the mechanical and electrical performances have to be consistent under different interface conditions, to ensure the accuracy and robustness of the devices. Here, the effect of interface conditions on the mechanical and electrical performances is studied for stretchable inorganic electronics with different configurations by theoretical analysis, finite element analysis and experiment. A universal size design principle is proposed for stretchable inorganic electronics to work consistently under different interface conditions, i.e., the period length of the devices/interconnects has to be the same order of magnitude as the encapsulation thickness or less. To ensure the comfort of human skin/organs, micron-scale geometrical design is necessary for epidermal electronics according to the above designed principle. This finding is of great significance for ensuring the accuracy and robustness of stretchable inorganic electronics in practical applications.     

Full 3D Printing of Stretchable Piezoresistive Sensor with Hierarchical Porosity and Multimodulus Architecture

A soft piezoresistive sensor with its unique characteristics, such as human skin, light weight, and multiple functions, yields a variety of possible practical applications to skin‐attachable electronics, human–machine interfaces, and electronic skins. However, conventional filler‐matrix piezoresistive sensors often suffer from unsatisfactory sensitivity or insufficient measurement range, as well as significant cross‐correlation between out‐of‐plane pressure and in‐plane extension. Here, a stretchable piezoresistive sensor (SPS) is realized by combining a hierarchically porous sensing element with a multimodulus device architecture via a full 3D printing process. As a result, the sensor exhibits high sensitivity (5.54 kPa^?1), large measurement range (from 10 Pa to 800 kPa), limited cross‐correlation, and excellent durability. Meanwhile, benefiting from the porous structure and mechanical mismatch design, which efficiently distributes the stress away from the sensing element, the device experiences only 7% resistance change at 50% stretching. This approach is employed to rapidly program and readily manufacture stylish, all‐in‐one, functional devices for various applications, demonstrating that the technique is promising for customized stretchable electronics.