Self‐Healing Materials

Self‐healing materials are able to partially or completely heal damage inflicted on them, e.g., crack formation; it is anticipated that the original functionality can be restored. This article covers the design and generic principles of self‐healing materials through a wide range of different material classes including metals, ceramics, concrete, and polymers. Recent key developments and future challenges in the field of self‐healing materials are summarised, and generic, fundamental material‐independent principles and mechanism are discussed and evaluated.     

Writing,Self‐Healing,and Self‐Erasing on Conductive Pressure‐Sensitive Adhesives

A simple strategy for enabling conductive pressure sensitive adhesives (PSAs) to work as light‐responsive materials is reported. Direct laser‐writing of PSA substrates was achieved by means of a continuous‐wave He‐Ne laser focused through the objectives of an optical microscope. This approach takes advantage of cooperative interplay between viscoelastic properties of PSAs and enhanced thermal conductivity provided by an extra overlayer of gold. In particular, the thickness of the gold layer is a crucial parameter for tuning the substrate responsiveness. Self‐healing and self‐degradation processes can be exploited for controlling the lifetime of the written information, whereas additional protective coatings can be introduced to achieve permanent storage.     

Self‐Healing Hydrogels

Over the past few years, there has been a great deal of interest in the development of hydrogel materials with tunable structural, mechanical, and rheological properties, which exhibit rapid and autonomous self‐healing and self‐recovery for utilization in a broad range of applications, from soft robotics to tissue engineering. However, self‐healing hydrogels generally either possess mechanically robust or rapid self‐healing properties but not both. Hence, the development of a mechanically robust hydrogel material with autonomous self‐healing on the time scale of seconds is yet to be fully realized. Here, the current advances in the development of autonomous self‐healing hydrogels are reviewed. Specifically, methods to test self‐healing efficiencies and recoveries, mechanisms of autonomous self‐healing, and mechanically robust hydrogels are presented. The trends indicate that hydrogels that self‐heal better also achieve self‐healing faster, as compared to gels that only partially self‐heal. Recommendations to guide future development of self‐healing hydrogels are offered and the potential relevance of self‐healing hydrogels to the exciting research areas of 3D/4D printing, soft robotics, and assisted health technologies is highlighted.     

Tough Self‐Healing Elastomers by Molecular Enforced Integration of Covalent and Reversible Networks

Self‐healing polymers crosslinked by solely reversible bonds are intrinsically weaker than common covalently crosslinked networks. Introducing covalent crosslinks into a reversible network would improve mechanical strength. It is challenging, however, to apply this concept to “dry” elastomers, largely because reversible crosslinks such as hydrogen bonds are often polar motifs, whereas covalent crosslinks are nonpolar motifs. These two types of bonds are intrinsically immiscible without cosolvents. Here, we design and fabricate a hybrid polymer network by crosslinking randomly branched polymers carrying motifs that can form both reversible hydrogen bonds and permanent covalent crosslinks. The randomly branched polymer links such two types of bonds and forces them to mix on the molecular level without cosolvents. This enables a hybrid “dry” elastomer that is very tough with fracture energy 13500 Jm^?2 comparable to that of natural rubber. Moreover, the elastomer can self‐heal at room temperature with a recovered tensile strength 4 MPa, which is 30% of its original value, yet comparable to the pristine strength of existing self‐healing polymers. The concept of forcing covalent and reversible bonds to mix at molecular scale to create a homogenous network is quite general and should enable development of tough, self‐healing polymers of practical usage.     

Synthetic Multifunctional Graphene Composites with Reshaping and Self‐Healing Features via a Facile Biomineralization‐Inspired Process

Since graphene is a type of 2D carbon material with excellent mechanical, electrical, thermal, and optical properties, the efficient preparation of graphene macroscopic assemblies is significant in the potentially large‐scale application of graphene sheets. Conventional preparation methods of graphene macroscopic assemblies need strict conditions, and, once formed, the assemblies cannot be edited, reshaped, or recycled. Herein, inspired by the biomineralization process, a feasible approach of shapeable, multimanipulatable, and recyclable gel‐like composite consisting of graphene oxide/poly(acrylic acid)/amorphous calcium carbonate (GO‐PAA‐ACC) is designed. This GO‐PAA‐ACC material can be facilely synthesized at room temperature with a cross‐linking network structure formed during the preparation process. Remarkably, it is stretchable, malleable, self‐healable, and easy to process in the wet state, but tough and rigid in the dried state. In addition, these two states can be readily switched by adjusting the water content, which shows recyclability and can be used for 3D printing to form varied architectures. Furthermore, GO‐PAA‐ACC can be functionalized or processed to meet a variety of specific application requirements (e.g., energy‐storage, actuators). The preparation method of GO‐PAA‐ACC composite in this work also provides a novel strategy for the versatile macroscopic assembly of other materials, which is low‐cost, efficient, and convenient for broad application.