Achieving cycling stability of silicon-based anodes for lithium-ion batteries: From lithium storage/failure mechanism to structure optimization

Abstract

Silicon-based materials are regarded as one of the key anode materials for high-performance Lithium-ion batteries (LIBs), based on the advantages of high theoretical specific capacity, low lithiation/delithiation potentials, and abundant reserves. However, the poor stability caused by their large volume effect and irreversible lithium recuperation caused by the formation of solid electrolyte layer (SEI) and electrical disconnection for LiSi particles, severely limit their further commercial application. Aiming at these problems and challenges faced by silicon-based materials, this review introduces the lithium storage mechanism and analyzes the material failure mechanism from the dimensions of electrochemical reaction deactivation and physical-electrical contact deactivation. From the perspectives of silicon-based materials and electrode structure design, the mechanical/electrochemical stability enhancement strategies of silicon-based material dimensions and carbon material composite structures are summarized in detail, and the modification mechanisms of multi-alloying and pre-lithiation are analyzed. Finally, the further commercial application of silicon-based materials is envisioned and its key development directions are discussed, emphasizing the practical significance of structural design with excellent mechanical properties and stable lithiation interfaces in the development of silicon‑carbon materials.