Inhibition of Structural Degradation in Silicon Anodes of Lithium-Ion Batteries Using a Supramolecular Self-Healing Binders based on a Host-Guest System

Abstract

Silicon (Si) is a promising anode material for lithium-ion batteries (LIBs) due to its high theoretical capacity. However, it suffers from severe volume expansion during cycling, leading to particle pulverization and unstable solid electrolyte interphase (SEI), which result in rapid capacity fading. Conventional binders such as PVDF and PAA have weak interactions with Si and cannot effectively suppress such degradation. In this study, we propose a novel self-healing polymeric binder based on supramolecular host–guest interactions to address this issue. The dynamic reversible bonds allow the binder to dissipate mechanical stress and autonomously heal cracks formed during cycling. As a result, the Si electrode maintains its structural integrity and electrochemical performance over extended cycles. Our findings demonstrate that supramolecular self-healing binders are a promising strategy for enhancing the durability of Si anodes and advancing high-capacity next-generation LIBs.