Energy Harvesters for Wearable and Stretchable Electronics: From Flexibility to Stretchability

The rapid advancements of wearable electronics have caused a paradigm shift in consumer electronics, and the emerging development of stretchable electronics opens a new spectrum of applications for electronic systems. Playing a critical role as the power sources for independent electronic systems, energy harvesters with high flexibility or stretchability have been the focus of research efforts over the past decade. A large number of the flexible energy harvesters developed can only operate at very low strain level (≈0.1%), and their limited flexibility impedes their application in wearable or stretchable electronics. Here, the development of highly flexible and stretchable (stretchability >15% strain) energy harvesters is reviewed with emphasis on strategies of materials synthesis, device fabrication, and integration schemes for enhanced flexibility and stretchability. Due to their particular potential applications in wearable and stretchable electronics, energy‐harvesting devices based on piezoelectricity, triboelectricity, thermoelectricity, and dielectric elastomers have been largely developed and the progress is summarized. The challenges and opportunities of assembly and integration of energy harvesters into stretchable systems are also discussed.     

Wearable Electronics Based on 2D Materials for Human Physiological Information Detection

Recently, advancement in materials production, device fabrication, and flexible circuit has led to the huge prosperity of wearable electronics for human healthcare monitoring and medical diagnosis. Particularly, with the emergence of 2D materials many merits including light weight, high stretchability, excellent biocompatibility, and high performance are used for those potential applications. Thus, it is urgent to review the wearable electronics based on 2D materials for the detection of various human signals. In this work, the typical graphene‐based materials, transition‐metal dichalcogenides, and transition metal carbides or carbonitrides used for the wearable electronics are discussed. To well understand the human physiological information, it is divided into two dominated categories, namely, the human physical and the human chemical signals. The monitoring of body temperature, electrograms, subtle signals, and limb motions is described for the physical signals while the detection of body fluid including sweat, breathing gas, and saliva is reviewed for the chemical signals. Recent progress and development toward those specific utilizations are highlighted in the Review with the representative examples. The future outlook of wearable healthcare techniques is briefly discussed for their commercialization.     

Advances in Rational Design and Materials of High‐Performance Stretchable Electromechanical Sensors

Stretchable and wearable sensor technology has attracted significant interests and created high technological impact on portable healthcare and smart human–machine interfaces. Wearable electromechanical systems are an important part of this technology that has recently witnessed tremendous progress toward high‐performance devices for commercialization. Over the past few years, great attention has been paid to simultaneously enhance the sensitivity and stretchability of the electromechanical sensors toward high sensitivity, ultra‐stretchability, low power consumption or self‐power functionalities, miniaturisation as well as simplicity in design and fabrication. This work presents state‐of‐the‐art advanced materials and rational designs of electromechanical sensors for wearable applications. Advances in various sensing concepts and structural designs for intrinsic stretchable conductive materials as well as advanced rational platforms are discussed. In addition, the practical applications and challenges in the development of stretchable electromechanical sensors are briefly mentioned and highlighted.     

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.     

Recent Advances in Transparent Electronics with Stretchable Forms

Advances in materials science and the desire for next‐generation electronics have driven the development of stretchable and transparent electronics in the past decade. Novel applications, such as smart contact lenses and wearable sensors, have been introduced with stretchable and transparent form factors, requiring a deeper and wider exploration of materials and fabrication processes. In this regard, many research efforts have been dedicated to the development of mechanically stretchable, optically transparent materials and devices. Recent advances in stretchable and transparent electronics are discussed herein, with special emphasis on the development of stretchable and transparent materials, including substrates and electrodes. Several representative examples of applications enabled by stretchable and transparent electronics are presented, including sensors, smart contact lenses, heaters, and neural interfaces. The current challenges and opportunities for each type of stretchable and transparent electronics are also discussed.     

Scalable Production of Wearable Solid-State Li-Ion Capacitors from N-Doped Hierarchical Carbon

Smart and wearable electronics have aroused substantial demand for flexible portable power sources, but it remains a large challenge to realize scalable production of wearable batteries/supercapacitors with high electrochemical performance and remarkable flexibility simultaneously. Here, a scalable approach is developed to prepare wearable solid-state lithium-ion capacitors (LICs) with superior performance enabled by synergetic engineering from materials to device architecture. Nitrogen-doped hierarchical carbon (HC) composed of 1D carbon nanofibers welded with 2D carbon nanosheets is synthesized via a unique self-propagating high-temperature synthesis (SHS) technique, which exhibits superior electrochemical performance. Subsequently, inspired by origami, here, wave-shaped LIC punch-cells based on the above materials are designed by employing a compatible and scalable post-imprint technology. Finite elemental analysis (FEA) confirms that the bending stress of the punch-cell can be offset effectively, benefiting from the wave architecture. The wearable solid-state LIC punch-cell exhibits large energy density, long cyclic stability, and superior flexibility. This study demonstrates great promise for scalable fabrication of wearable energy-storage systems.     

Flexible Sensing Electronics for Wearable/Attachable Health Monitoring

Wearable or attachable health monitoring smart systems are considered to be the next generation of personal portable devices for remote medicine practices. Smart flexible sensing electronics are components crucial in endowing health monitoring systems with the capability of real‐time tracking of physiological signals. These signals are closely associated with body conditions, such as heart rate, wrist pulse, body temperature, blood/intraocular pressure and blood/sweat bio‐information. Monitoring such physiological signals provides a convenient and non‐invasive way for disease diagnoses and health assessments. This Review summarizes the recent progress of flexible sensing electronics for their use in wearable/attachable health monitoring systems. Meanwhile, we present an overview of different materials and configurations for flexible sensors, including piezo‐resistive, piezo‐electrical, capacitive, and field effect transistor based devices, and analyze the working principles in monitoring physiological signals. In addition, the future perspectives of wearable healthcare systems and the technical demands on their commercialization are briefly discussed.     

Recent Progress of Fiber Shaped Lighting Devices for Smart Display Applications—A Fibertronic Perspective

Advances in material science and nanotechnology have fostered the miniaturization of devices. Over the past two decades, the form-factor of these devices has evolved from 3D rigid, volumetric devices through 2D film-based flexible electronics, finally to 1D fiber electronics (fibertronics). In this regard, fibertronic strategies toward wearable applications (e.g., electronic textiles (e-textiles)) have attracted considerable attention thanks to their capability to impart various functions into textiles with retaining textiles' intrinsic properties as well as imperceptible irritation by foreign matters. In recent years, extensive research has been carried out to develop various functional devices in the fiber form. Among various features, lighting and display features are the highly desirable functions in wearable electronics. This article discusses the recent progress of materials, architectural designs, and new fabrication technologies of fiber-shaped lighting devices and the current challenges corresponding to each device's operating mechanism. Moreover, opportunities and applications that the revolutionary convergence between the state-of-the-art fibertronic technology and age-long textile industry will bring in the future are also discussed.     

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.     

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.     

A New Facile Route to Flexible and Semi‐Transparent Electrodes Based on Water Exfoliated Graphene and their Single‐Electrode Triboelectric Nanogenerator

Wearable technologies are driving current research efforts to self‐powered electronics, for which novel high‐performance materials such as graphene and low‐cost fabrication processes are highly sought.The integration of high‐quality graphene films obtained from scalable water processing approaches in emerging applications for flexible and wearable electronics is demonstrated. A novel method for the assembly of shear exfoliated graphene in water, comprising a direct transfer process assisted by evaporation of isopropyl alcohol is developed. It is shown that graphene films can be easily transferred to any target substrate such as paper, flexible polymeric sheets and fibers, glass, and Si substrates. By combining graphene as the electrode and poly(dimethylsiloxane) as the active layer, a flexible and semi‐transparent triboelectric nanogenerator (TENG) is demonstrated for harvesting energy. The results constitute a new step toward the realization of energy harvesting devices that could be integrated with a wide range of wearable and flexible technologies, and opens new possibilities for the use of TENGs in many applications such as electronic skin and wearable electronics.     

Printable Fabrication of Nanocoral‐Structured Electrodes for High‐Performance Flexible and Planar Supercapacitor with Artistic Design

Planar supercapacitors with high flexibility, desirable operation safety, and high performance are considered as attractive candidates to serve as energy‐storage devices for portable and wearable electronics. Here, a scalable and printable technique is adopted to construct novel and unique hierarchical nanocoral structures as the interdigitated electrodes on flexible substrates. The as‐fabricated flexible all‐solid‐state planar supercapacitors with nanocoral structures achieve areal capacitance up to 52.9 mF cm^?2, which is 2.5 times that of devices without nanocoral structures, and this figure‐of‐merit is among the highest in the literature for the same category of devices. More interestingly, due to utilization of the inkjet‐printing technique, excellent versatility on electrode‐pattern artistic design is achieved. Particularly, working supercapacitors with artistically designed patterns are demonstrated. Meanwhile, the high scalability of such a printable method is also demonstrated by fabrication of large‐sized artistic supercapacitors serving as energy‐storage devices in a wearable self‐powered system as a proof of concept.     

Stable and Biocompatible Carbon Nanotube Ink Mediated by Silk Protein for Printed Electronics

Ink-based processes, which enable scalable fabrication of flexible devices based on nanomaterials, are one of the practical approaches for the production of wearable electronics. However, carbon nanotubes (CNTs), which possess great potential for flexible electronics, are facing challenges for use in inks due to their low dispersity in most solvents and suspicious cytotoxicity. Here, a stable and biocompatible CNT ink, which is stabilized by sustainable silk sericin and free from any artificial chemicals, is reported. The ink shows stability up to months, which can be attributed to the formation of sericin–CNT (SSCNT) hybrid through non-covalent interactions. It is demonstrated that the SSCNT ink can be used for fabricating versatile circuits on textile, paper, and plastic films through various techniques. As proofs of concept, electrocardiogram electrodes, breath sensors, and electrochemical sensors for monitoring human health and activity are fabricated, demonstrating the great potential of the SSCNT ink for smart wearables.     

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.     

Buckled Structures: Fabrication and Applications in Wearable Electronics

Wearable electronics have attracted a tremendous amount of attention due to their many potential applications, such as personalized health monitoring, motion detection, and smart clothing, where electronic devices must conformably form contacts with curvilinear surfaces and undergo large deformations. Structural design and material selection have been the key factors for the development of wearable electronics in the recent decades. As one of the most widely used geometries, buckling structures endow high stretchability, high mechanical durability, and comfortable contact for human–machine interaction via wearable devices. In addition, buckling structures that are derived from natural biosurfaces have high potential for use in cost‐effective and high‐grade wearable electronics. This review provides fundamental insights into buckling fabrication and discusses recent advancements for practical applications of buckled electronics, such as interconnects, sensors, transistors, energy storage, and conversion devices. In addition to the incorporation of desired functions, the simple and consecutive manipulation and advanced structural design of the buckled structures are discussed, which are important for advancing the field of wearable electronics. The remaining challenges and future perspectives for buckled electronics are briefly discussed in the final section.     

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.     

Polymer‐Assisted Metal Deposition (PAMD) for Flexible and Wearable Electronics: Principle,Materials, Printing,and Devices

The rapid development of flexible and wearable electronics favors low‐cost, solution‐processing, and high‐throughput techniques for fabricating metal contacts, interconnects, and electrodes on flexible substrates of different natures. Conventional top‐down printing strategies with metal‐nanoparticle‐formulated inks based on the thermal sintering mechanism often suffer from overheating, rough film surface, low adhesion, and poor metal quality, which are not desirable for most flexible electronic applications. In recent years, a bottom‐up strategy termed as polymer‐assisted metal deposition (PAMD) shows great promise in addressing the abovementioned challenges. Here, a detailed review of the development of PAMD in the past decade is provided, covering the fundamental chemical mechanism, the preparation of various soft and conductive metallic materials, the compatibility to different printing technologies, and the applications for a wide variety of flexible and wearable electronic devices. Finally, the attributes of PAMD in comparison with conventional nanoparticle strategies are summarized and future technological and application potentials are elaborated.     

A New Frontier of Printed Electronics: Flexible Hybrid Electronics

The performance and integration density of silicon integrated circuits (ICs) have progressed at an unprecedented pace in the past 60 years. While silicon ICs thrive at low-power high-performance computing, creating flexible and large-area electronics using silicon remains a challenge. On the other hand, flexible and printed electronics use intrinsically flexible materials and printing techniques to manufacture compliant and large-area electronics. Nonetheless, flexible electronics are not as efficient as silicon ICs for computation and signal communication. Flexible hybrid electronics (FHE) leverages the strengths of these two dissimilar technologies. It uses flexible and printed electronics where flexibility and scalability are required, i.e., for sensing and actuating, and silicon ICs for computation and communication purposes. Combining flexible electronics and silicon ICs yields a very powerful and versatile technology with a vast range of applications. Here, the fundamental building blocks of an FHE system, printed sensors and circuits, thinned silicon ICs, printed antennas, printed energy harvesting and storage modules, and printed displays, are discussed. Emerging application areas of FHE in wearable health, structural health, industrial, environmental, and agricultural sensing are reviewed. Overall, the recent progress, fabrication, application, and challenges, and an outlook, related to FHE are presented.     

An Overview of the Development of Flexible Sensors

Flexible sensors that efficiently detect various stimuli relevant to specific environmental or biological species have been extensively studied due to their great potential for the Internet of Things and wearable electronics applications. The application of flexible and stretchable electronics to device‐engineering technologies has enabled the fabrication of slender, lightweight, stretchable, and foldable sensors. Here, recent studies on flexible sensors for biological analytes, ions, light, and pH are outlined. In addition, contemporary studies on device structure, materials, and fabrication methods for flexible sensors are discussed, and a market overview is provided. The conclusion presents challenges and perspectives in this field.     

Recent Advances in Wearable Transdermal Delivery Systems

Wearable transdermal delivery systems have recently received tremendous attention due to their noninvasive, convenient, and prolonged administration of pharmacological agents. Here, the material prospects, fabrication processes, and drug‐release mechanisms of these types of therapeutic delivery systems are critically reviewed. The latest progress in the development of multifunctional wearable devices capable of closed‐loop sensation and drug delivery is also discussed. This survey reveals that wearable transdermal delivery has already made an impact in diverse healthcare applications, while several grand challenges remain.