LAUSR

Advanced rechargeable lithium-based batteries have a profound effect on our global society and polymer materials are one of the key components of these batteries. The key roles of polymers applied in battery technology are presented in terms of binders, package coatings, separators, and electrolytes. However, the loathsomely structural changes during repeated charge/discharge processes result in the mechanical fracture problems of polymers inside batteries, which significantly reduce the cycling lifetimes. The use of intrinsic self-healing polymers as substitutes is one of the most favored strategies for reviving lithium-based batteries since self-healing polymers spontaneously eliminate the mechanical cracks or damages and result in greatly enhanced electrochemical performances. In this review, we first introduce the advances and working mechanism of intrinsic self-healing polymers. Then, we discuss the opportunities and challenges in the development of advanced lithium-based batteries with Si, Li-metal, S electrodes, and polymer electrolytes, respectively, and summarize the up-to-date key progress in intrinsic self-healing polymers for solving the above-mentioned challenges. Finally, we propose some designing principles of desired intrinsic self-healing polymers from the perspectives of basic structures, ionic conductivities, mechanical properties, chemical interactions, and the self-healing capabilities.