Revitalizing Micro‐Sized Si‐Based Anodes Through Advanced Structural Design and Interface Stabilization: A Review

Silicon (Si) is recognized as a promising anode material for next-generation lithium-ion batteries owing to its exceptionally high lithium storage capacity. Recently, micro-sized Si (micro-Si) based anodes have re-emerged as alternatives to nano-sized Si (nano-Si) owing to their higher tap density and reduced interfacial side reactions. Considerable efforts are devoted to addressing the rapid capacity decay caused by severe volume expansion, sluggish kinetics, and continuous accumulation of the solid electrolyte interphase. In this review, the primary failure mechanisms of micro-Si anodes is first analyzed and subsequently summarize recent advances in enhancing their structural and interfacial stability. The design of Si-containing materials (primarily Si/C composites and SiO_x structures) that meet the current industrial requirements is discussed. Additionally, binder optimization and electrolyte exploration are analyzed. Finally, the potential application of advanced spectroscopic, electronic, and mechanical characterization techniques is explored, coupled with machine learning, in developing Si-based anodes. This review aims to comprehensively understand the rational design and in-depth analysis of next-generation micro-Si based lithium-ion batteries.