Toward interface-adaptive silicon anodes: From 3D SEI to dynamic coupled interphases.

This review examines the development of silicon anodes in lithium-ion batteries, focusing on modifying the solid electrolyte interphase (SEI) to address issues arising from silicon's significant volume expansion. It promotes a transition from static, stabilizing strategies to dynamic, adaptive interfaces that evolve in accordance with silicon's behavior during cycling. The discussion highlights key advancements in the dimensional evolution of SEI layers, transitioning from brittle 3D structures to more stable, conductive 2D configurations. The significance of hierarchical chemical coupling, integrating rigid inorganic components such as LiF with flexible polymer matrices, is highlighted for its role in ensuring mechanical stability and ionic conductivity. The integration of self-healing strategies and dynamic chemical bonds and the system-level integration of electrolytes, electrodes, and interfaces are critical for developing intelligent silicon anodes capable of adapting to mechanical and electrochemical stresses. This novel approach has the potential to enhance the performance and longevity of silicon-based anodes in next-generation batteries.