Conducting polymer hydrogels have been employed in diverse fields such as energy storage and bioelectronics, which possess both the mechanical properties of hydrogels and electronic transport properties of conducting polymers. However, the rigid and fragile nature of conducting polymers hinders the long-time stability of the hydrogels and limits their applications in emerging flexible electronic devices. In this work, we have developed a novel type of multifunctional conductive polymer hydrogel, of which high conductivity is integrated with excellent stretchability, injectability, and rapid self-healing capability, by incorporating multiple hydrogen-bonding 2-ureido-4­[1H]-pyrimidinone (UPy) groups as cross-linking points into a brittle polyaniline/poly­(4-styrenesulfonate) (PANI/PSS) network. The formation of the interpenetrating PANI/PSS network offers the hydrogel electronic conduction assisted by ionic transport, showing a conductivity of 13 S/m and a linear response (gauge factor = 3.4) to external strain (≈300%), with accurate and reliable detection of various human motions. Taking advantage of the reversibility of the noncovalent cross-links, the hydrogels can be facilely molded into different shapes and demonstrate a complete self-healing within 30 s upon damage. The combination of supramolecular chemistry with conducting polymers enables multifunctionalities in the conductive hydrogel, providing new insights into the design of advanced functional materials with applications in 3D printing, wearable devices, and flexible electronics.

This review article gives an overview of the molecular adhesion mechanisms and recent development of mussel inspired functional adhesives.

Flexible electronics have emerged as an exciting research area in recent years, serving as ideal interfaces bridging biological systems and conventional electronic devices. Flexible electronics can not only collect physiological signals for human health monitoring but also enrich our daily life with multifunctional smart materials and devices. Conductive hydrogels (CHs) have become promising candidates for the fabrication of flexible electronics owing to their biocompatibility, adjustable mechanical flexibility, good conductivity, and multiple stimuli‐responsive properties. To achieve on‐demand mechanical properties such as stretchability, compressibility, and elasticity, the rational design of polymer networks via modulating chemical and physical intermolecular interactions is required. Moreover, the type of conductive components (eg, electron‐conductive materials, ions) and the incorporation method also play an important role in the conductivity of CHs. Electron‐CHs usually possess excellent conductivity, while ion‐CHs are generally transparent and can generate ion gradients within the hydrogel matrices. This mini review focuses on the recent advances in the design of CHs, introducing various design strategies for electron‐CHs and ion‐CHs employed in flexible electronics and highlighting their versatile applications such as biosensors, batteries, supercapacitors, nanogenerators, actuators, touch panels, and displays.image

Although recent years have witnessed intense efforts and innovations in the design of flexible conductive materials for the development of next-generation electronic devices, it remains a great challenge to integrate multifunctionalities such as stretchability, self-healing, adhesiveness, and sensing capability into one conductive system for practical applications. In this work, for the first time, we have prepared a new electrically conductive elastomer composite that combines all these functionalities by triggering in situ polymerization of pyrrole in a supramolecular polymer matrix cross-linked by multiple hydrogen-bonding 2-ureido-4­[1H]-pyrimidinone (UPy) groups. The polypyrrole (PPy) particles were uniformly dispersed and imparted to the composite desirable conductive properties, while the reversible nature of the dynamic multiple hydrogen bonds in the polymer matrix allowed excellent stretchability, fast self-healing ability, and adhesiveness under ambient condition. The elastomer composite with the incorporation of 7.5 wt % PPy displayed a mechanical strength of 0.72 MPa with an elongation over 300%, where the rapid self-healing of the mechanical and electrical properties was achieved within 5 min. The elastic material also exhibited strong adhesiveness to a broad range of inorganic and organic substrates, and it was further fabricated as a strain sensor for the detection of both large and subtle human motions (i.e., finger bending, pulse beating). The novel PPy-doped conductive elastomer has demonstrated great potential as functional sensors for wearable electronics, which provides a facile and promising approach to the development of various flexible electronic materials with multifunctionalities by combining conductive components with supramolecular polymers.

A self-healing hydrogel ionic conductor has been developed by combining dynamic covalent chemistry with nanofiller reinforcement and micelle crosslinking, and used for sensing of diverse human activities.