Application of silicon‐based anode is significantly challenged by low initial Coulombic efficiency (ICE) and poor cyclability. Traditional pre‐lithiation reagents often pose safety concerns due to their unstable chemical nature. Achieving a balance between water‐stability and high ICE in prelithiated silicon is a critical issue. Here, we present a lithium‐enriched silicon/graphite material with an ultra‐high ICE of ≥110% through a high‐stable lithium pre‐storage methodology. Lithium pre‐storage prepared a nano‐drilled graphite material with surficial lithium functional groups, which can form chemical bonds with adjacent silicon during high‐temperature sintering. This results in an unexpected O‐Li‐Si interaction, leading to in‐situ pre‐lithiation of silicon nanoparticles and providing high stability characteristics in air and water. Additionally, the lithium‐enriched silicon/graphite materials impart a combination of high ICE, high specific capacity (620 mAh g‐1), and long cycling stability (> 400 cycles). This study opens up a promising avenue for highly air and water‐stable silicon anode prelithiation methods.

中文翻译：

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锂预存储可实现高初始库仑效率和稳定的富锂硅/石墨阳极

硅基阳极的应用受到初始库仑效率（ICE）低和循环性能差的严重挑战。传统的预锂化试剂由于其不稳定的化学性质经常引起安全问题。在预锂化硅中实现水稳定性和高 ICE 之间的平衡是一个关键问题。在这里，我们通过高稳定的锂预存储方法提出了一种富锂硅/石墨材料，其 ICE ≥110%。锂预储存制备了表面带有锂官能团的纳米钻孔石墨材料，在高温烧结过程中可以与相邻的硅形成化学键。这导致了意想不到的 O-Li-Si 相互作用，导致硅纳米粒子的原位预锂化，并在空气和水中提供高稳定性特性。此外，富锂硅/石墨材料还具有高 ICE、高比容量（620 mAh g-1）和长循环稳定性（> 400 次循环）的组合。这项研究为空气和水高度稳定的硅阳极预锂化方法开辟了一条有前途的途径。