The Polymer Society of Korea

Abstract

Lithium (Li) metal offers the highest theoretical capacity and lowest electrochemical potential among anode materials, but practical use is hindered by unstable interfacial chemistry causing dendrite formation and capacity loss. We introduce fully grafted bottlebrush polymers (BBPs) with polynorbornene backbones and lithiophilic polyethylene glycol side chains as artificial solid electrolyte interphases (SEIs). By varying backbone and side-chain lengths, we elucidated how molecular entanglement governs mechanical resilience and ion coordination of polymer interphases. The optimized BBP forms an entangled network that resists electrolyte swelling and promotes uniform Li deposition. Comprehensive analyses confirm the essential role of architecture-driven entanglement in establishing stable SEIs. This work establishes a molecular design strategy leveraging polymer entanglement to achieve durable, high-efficiency Li metal anodes.