Lithium Hydride in the Solid Electrolyte Interphase of Lithium‐Ion Batteries as a Pulverization Accelerator of Silicon

As a highly promising next-generation high-specific capacity anode, the industrial-scale utilization of micron silicon has been hindered by the issue of pulverization during cycling. Although numerous studies have demonstrated the effectiveness of regulating the inorganic components of the solid electrolyte interphase (SEI) in improving pulverization, the evolution of most key inorganic components in the SEI and their correlation with silicon failure mechanisms remain ambiguous. This study provides a clear and direct correlation between the lithium hydride (LiH) in the SEI and the degree of micron silicon pulverization in the battery system. The reverse lithiation behavior of LiH on micron silicon during de-lithiation exacerbates the localized stress in silicon particles and contributes to particle pulverization. This work successfully proposes a novel approach to decouple the SEI from electrochemical performance, which can be significant to decipher the evolution of critical SEI components at varied battery anode interfaces and analyze their corresponding failure mechanisms.