Engineering Nanostructure, Interface, and Prelithiation of Advanced Silicon-Based Lithium-Ion Battery Anodes

Silicon (Si) has emerged as a leading candidate to replace traditional graphite anodes in the next generation of high-energy-density lithium-ion batteries, owing to its exceptionally high theoretical capacity, favorable working voltage, natural abundance, and environmental friendliness. However, substantial challenges, including poor electrical and ionic conductivity, considerable volume changes, and an unstable solid-electrolyte interphase, impede its commercial adoption. To overcome these barriers, various material optimization strategies have been developed for the synthesis of Si-based composites. This review meticulously details recent advancements and prospective studies on Si-based composites, highlighting progress in nanocomposite synthesis strategies, interface adjustments, and advanced prelithiation techniques aimed at enhancing the electrochemical performance of Si-based composite anodes. Special emphasis is placed on the Li–Si alloy storage mechanism, structural and chemical evolution at the Si anode/electrolyte interface, and precise prelithiation regulation. Finally, the practical application of Si-based anodes is discussed, providing feasible reference solutions for the development of high-performance Si-based anodes.