Controlled radical polymerization-derived solid-state polymer electrolytes for lithium batteries

Solid-state polymer electrolytes (SPEs) have emerged as a promising candidate to work out remaining challenges faced by conventional liquid electrolytes, including the safety risks and limited energy density lithium batteries. Despite these benefits, polymer electrolytes are still required further optimization for constructing high-performance energy storage systems. Controlled radical polymerization (CRP) techniques, encompassing reversible addition-fragmentation transfer (RAFT), atom transfer radical polymerization (ATRP), and nitroxide-mediated polymerization (NMP), enable precise control over polymer architectures, molecular weights, and functionalities, which plays an essential role in regulating the ionic conductivity, cycling stability, mechanical performance, and interfacial compatibility of polymer electrolytes. Here, on the basis of discussing the CRP reaction mechanisms and the typical topological structures, this review thoroughly delves into the effects of CRP on electrochemical performance, and particularly focuses the current development of polymer electrolytes with different topological structures synthesized via CRP. Ending with providing the underlying challenges and perspectives, this review allows to deepen the comprehension of CRP methodologies on constructing polymer electrolytes, and offers the scientific guidance for shaping the high-performance CRP-derived polymer electrolytes.