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Stretchable electronics have increasingly gained interest both in the academic and industrial communities owing to its potential to enable a wide variety of applications, especially ...wearable and implantable devices for biomedical applications. As the key component for electronic devices, the design of a suitable semiconductor is essential, while the solution processability and structural tunability of polymer semiconductor make it a promising candidate. Along this line, it is important to consider the mechanical properties of polymer semiconductors in the design of flexible and stretchable devices placed on soft and curved surfaces to accommodate the constant movement of the human body. However, achieving high mechanical deformability and high charge transport properties simultaneously in polymer semiconductors remains a major challenge. In this trend article, we survey various approaches in designing intrinsically stretchable conjugated polymers, focusing on structure-property relationships from a molecular perspective, such as molecular weight, regioregularity, backbone and side chain modifications. Understanding the influence of these molecular structure parameters on thin film morphology may provide general guidelines for achieving desired microstructures that allow mechanical deformation without interrupting charge transport. Beyond highlighting recent key work in this field, we will discuss future prospects of stretchable conjugated polymers.
Conspectus Future electronics will take on more important roles in people’s lives. They need to allow more intimate contact with human beings to enable advanced health monitoring, disease detection, ...medical therapies, and human–machine interfacing. However, current electronics are rigid, nondegradable and cannot self-repair, while the human body is soft, dynamic, stretchable, biodegradable, and self-healing. Therefore, it is critical to develop a new class of electronic materials that incorporate skinlike properties, including stretchability for conformable integration, minimal discomfort and suppressed invasive reactions; self-healing for long-term durability under harsh mechanical conditions; and biodegradability for reducing environmental impact and obviating the need for secondary device removal for medical implants. These demands have fueled the development of a new generation of electronic materials, primarily composed of polymers and polymer composites with both high electrical performance and skinlike properties, and consequently led to a new paradigm of electronics, termed “skin-inspired electronics”. This Account covers recent important advances in skin-inspired electronics, from basic material developments to device components and proof-of-concept demonstrations for integrated bioelectronics applications. To date, stretchability has been the most prominent focus in this field. In contrast to strain-engineering approaches that extrinsically impart stretchability into inorganic electronics, intrinsically stretchable materials provide a direct route to achieve higher mechanical robustness, higher device density, and scalable fabrication. The key is the introduction of strain-dissipation mechanisms into the material design, which has been realized through molecular engineering (e.g., soft molecular segments, dynamic bonds) and physical engineering (e.g., nanoconfinement effect, geometric design). The material design concepts have led to the successful demonstrations of stretchable conductors, semiconductors, and dielectrics without sacrificing their electrical performance. Employing such materials, innovative device design coupled with fabrication method development has enabled stretchable sensors and displays as input/output components and large-scale transistor arrays for circuits and active matrixes. Strategies to incorporate self-healing into electronic materials are the second focus of this Account. To date, dynamic intermolecular interactions have been the most effective approach for imparting self-healing properties onto polymeric electronic materials, which have been utilized to fabricate self-healing sensors and actuators. Moreover, biodegradability has emerged as an important feature in skin-inspired electronics. The incorporation of degradable moieties along the polymer backbone allows for degradable conducting polymers and the use of bioderived materials has led to the demonstration of biodegradable functional devices, such as sensors and transistors. Finally, we highlight examples of skin-inspired electronics for three major applications: prosthetic e-skins, wearable electronics, and implantable electronics.
Conductive and stretchable materials that match the elastic moduli of biological tissue (0.5-500 kPa) are desired for enhanced interfacial and mechanical stability. Compared with inorganic and dry ...polymeric conductors, hydrogels made with conducting polymers are promising soft electrode materials due to their high water content. Nevertheless, most conducting polymer-based hydrogels sacrifice electronic performance to obtain useful mechanical properties. Here we report a method that overcomes this limitation using two interpenetrating hydrogel networks, one of which is formed by the gelation of the conducting polymer PEDOT:PSS. Due to the connectivity of the PEDOT:PSS network, conductivities up to 23 S m
are achieved, a record for stretchable PEDOT:PSS-based hydrogels. Meanwhile, the low concentration of PEDOT:PSS enables orthogonal control over the composite mechanical properties using a secondary polymer network. We demonstrate tunability of the elastic modulus over three biologically relevant orders of magnitude without compromising stretchability ( > 100%) or conductivity ( > 10 S m
).
There is an increasing demand for specialized pressure sensors in various applications. Previously, capacitive pressure sensors have been shown to have wide versatility in use, with a high degree of ...potential tuning possible through manipulating the geometry or material selection of the dielectric layer. However, in order to make sensors that are tunable and predictable, the design and fabrication method first needs to be developed. Presented here is an improved fabrication method to achieve tunable, consistent, and reproducible pressure sensors by using a pyramid microstructured dielectric layer along with a lamination layer. The as‐produced sensor performance is able to match predicted trends. Further, a simple model based on this system is developed and its efficacy is experimentally confirmed. Then, the model to predict a wide range of material and microstructure geometric properties prior to device fabrication is used to provide trends on sensor performance. Finally, it is demonstrated that the new method can be used to targetedly design a pressure sensor for a specific application—in vitro pulse sensing.
Tunable pressure sensors are achievable by geometric manipulation or material selection. To achieve this, tunable and reproducible pressure sensors are fabricated and modeled using a simple model based on microstructure properties. The model can be used to predict the effects of a wide range of material properties on sensor performance. Using this, targeted sensors for specific applications can be achieved.
Biodegradable electronics have great potential to reduce the environmental footprint of devices and enable advanced health monitoring and therapeutic technologies. Complex biodegradable electronics ...require biodegradable substrates, insulators, conductors, and semiconductors, all of which comprise the fundamental building blocks of devices. This review will survey recent trends in the strategies used to fabricate biodegradable forms of each of these components. Polymers that can disintegrate without full chemical breakdown (type I), as well as those that can be recycled into monomeric and oligomeric building blocks (type II), will be discussed. Type I degradation is typically achieved with engineering and material science based strategies, whereas type II degradation often requires deliberate synthetic approaches. Notably, unconventional degradable linkages capable of maintaining long-range conjugation have been relatively unexplored, yet may enable fully biodegradable conductors and semiconductors with uncompromised electrical properties. While substantial progress has been made in developing degradable device components, the electrical and mechanical properties of these materials must be improved before fully degradable complex electronics can be realized.
Due to their high water content and macroscopic connectivity, hydrogels made from the conducting polymer PEDOT:PSS are a promising platform from which to fabricate a wide range of porous conductive ...materials that are increasingly of interest in applications as varied as bioelectronics, regenerative medicine, and energy storage. Despite the promising properties of PEDOT:PSS‐based porous materials, the ability to pattern PEDOT:PSS hydrogels is still required to enable their integration with multifunctional and multichannel electronic devices. In this work, a novel electrochemical gelation (“electrogelation”) method is presented for rapidly patterning PEDOT:PSS hydrogels on any conductive template, including curved and 3D surfaces. High spatial resolution is achieved through use of a sacrificial metal layer to generate the hydrogel pattern, thereby enabling high‐performance conducting hydrogels and aerogels with desirable material properties to be introduced into increasingly complex device architectures.
PEDOT:PSS hydrogels are an important framework for creating conductive porous materials that are of broad interest to researchers in the fields of bioelectronics, tissue engineering, stretchable electronics, and energy. To incorporate these materials into devices, a novel patterning method is presented that uses electrochemically produced ions to rapidly generate PEDOT:PSS hydrogel patterns with high spatial resolution.
Through advances in molecular design, understanding of processing parameters, and development of non‐traditional device fabrication techniques, the field of wearable and implantable skin‐inspired ...devices is rapidly growing interest in the consumer market. Like previous technological advances, economic growth and efficiency is anticipated, as these devices will enable an augmented level of interaction between humans and the environment. However, the parallel growing electronic waste that is yet to be addressed has already left an adverse impact on the environment and human health. Looking forward, it is imperative to develop both human‐ and environmentally‐friendly electronics, which are contingent on emerging recyclable, biodegradable, and biocompatible polymer technologies. This review provides definitions for recyclable, biodegradable, and biocompatible polymers based on reported literature, an overview of the analytical techniques used to characterize mechanical and chemical property changes, and standard policies for real‐life applications. Then, various strategies in designing the next‐generation of polymers to be recyclable, biodegradable, or biocompatible with enhanced functionalities relative to traditional or commercial polymers are discussed. Finally, electronics that exhibit an element of recyclability, biodegradability, or biocompatibility with new molecular design are highlighted with the anticipation of integrating emerging polymer chemistries into future electronic devices.
With the rapid growth of consumer electronics, their harmonious integration into modern society and the environment is contingent on new eco‐ and human‐friendly polymer technologies. This review explores emerging recyclable, biodegradable, and biocompatible polymer chemistries with a focus on molecular design for incorporation into the next‐generation of sustainable electronics with unrealized capabilities.
Conjugation breakers (CBs) with different H-bonding chemistries and linker flexibilities are designed and incorporated into a diketopyrrolopyrrole (DPP)-based conjugated polymer backbone. The effects ...of H-bonding interactions on polymer semiconductor morphology, mechanical properties, and electrical performance are systematically investigated. We observe that CBs with an H-bonding self-association constant >0.7 or a denser packing tendency are able to induce higher polymer chain aggregation and crystallinity in as-casted thin films, resulting in a higher modulus and crack on-set strain. Additionally, the rDoC (relative degree of crystallinity) of the stretched thin film with the highest crack on-set strain only suffers a small decrease, suggesting the main energy dissipation mechanism is the breakage of H-bonding interactions. By contrast, other less stretchable polymer films dissipate strain energy through the breakage of crystalline domains, indicated by a drastic decrease in rDoC. Furthermore, we evaluate their electrical performances under mechanical strain in fully stretchable field-effect transistors. The polymer with the highest crack on-set strain has the least degradation in mobility as a function of strain. Overall, these observations suggest that we can aptly tune the mechanical properties of a polymer semiconductor by modulating intermolecular interactions, such as H-bonding chemistry and linker flexibility. Such understanding provides molecular design guidelines for future stretchable semiconductors.
Abstract
Intrinsically and fully stretchable active-matrix-driven displays are an important element to skin electronics that can be applied to many emerging fields, such as wearable electronics, ...consumer electronics and biomedical devices. Here, we show for the first time a fully stretchable active-matrix-driven organic light-emitting electrochemical cell array. Briefly, it is comprised of a stretchable light-emitting electrochemical cell array driven by a solution-processed, vertically integrated stretchable organic thin-film transistor active-matrix, which is enabled by the development of chemically-orthogonal and intrinsically stretchable dielectric materials. Our resulting active-matrix-driven organic light-emitting electrochemical cell array can be readily bent, twisted and stretched without affecting its device performance. When mounted on skin, the array can tolerate to repeated cycles at 30% strain. This work demonstrates the feasibility of skin-applicable displays and lays the foundation for further materials development.
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