Supramolecular interaction chemistry in polymer electrolytes towards stable lithium metal batteries

Developing advanced polymer electrolytes in lithium metal batteries (LMBs) has gained significant attention because of their inherent safety advantages over liquid electrolytes, while still encountering great challenges in mitigating uneven lithium plating/stripping and dendrite growth. Previous efforts primarily focused on passive approaches to mechanically constrain lithium dendrite growth. Recent studies have revealed the significance and effectiveness of regulating supramolecular interactions between polymer chains and other electrolyte components for homogenizing lithium deposition and enhancing the interfacial stability. This report provides a timely critical review to cover recent inspiring advancements in this direction. We first summarize the origins of supramolecular interaction origins, strength-determining factors, and structure–property relationships to establish quantitative correlations between polymer composition and supramolecular interaction properties. Then the recent advances in regulating supramolecular interaction chemistry are comprehensively discussed, focusing on those towards accelerated mass transport and stabilized anode-electrolyte interface. Finally, the remaining challenges are highlighted, and potential future directions in supramolecular interaction regulation of polymer electrolytes are prospected for the practical application of LMBs.