Applications of Dynamic Polymers in Next-Generation High-Performance Lithium-Based Batteries.

Abstract

Dynamic polymers, featuring reversible networks enabled by dynamic covalent bonds or non-covalent interactions, exhibit functionalities such as self-healing, reprocessability, mechanical adaptability, and recyclability. These attributes offer innovative material platforms to address critical challenges in next-generation high-performance lithium-based batteries (LBBs), including unstable solid-solid interfaces, the trade-off between mechanical robustness and ionic conductivity, and battery sustainability. This review summarizes recent advances in the design strategies, working mechanisms, and electrochemical performance of dynamic polymers for three major fields of LBBs: polymer electrolyte design, interface engineering, and binder development. By summarizing the relationships among dynamic bond chemistry (e.g., hydrogen bonds, disulfide, boronate ester, and imine bonds), network dynamics, and functional performance, we highlight the unique roles of dynamic polymers in improving interfacial stability, suppressing lithium dendrite growth, accommodating electrode volume changes, and enabling closed-loop recycling of battery components. Finally, we outline existing challenges and future research directions of the application of dynamic polymers toward the realization of high-energy-density, long-cycle-life, safe, and sustainable LBBs, providing insightful perspectives for the rational design of smart and eco-friendly battery materials.