Low-temperature de-alloying and unique self-filling interface optimization mechanism of layered silicon for enhanced lithium storage.

ABSTRACT

Layered silicon (L-Si) anodes are celebrated for their high theoretical capacity but face significant challenges regarding safety and material purity during preparation. This study addresses these challenges by employing NH4Cl-CaSi2 as the raw material in a gas-solid de-alloying process, which enhances both safety and purity compared to traditional methods. The L-Si anodes produced demonstrate outstanding electrochemical performance, delivering a high reversible lithium storage capacity of 1497.7 mA h g-1 at a current density of 0.5 A g-1, and exhibiting stable performance over 1200 charge-discharge cycles. In situ and ex situ characterizations reveal that electrolyte decomposition products effectively fill the voids within the electrode, while the gradual disintegration of the L-Si structure contributes to the formation of a dense, conductive network. This process enhances lithium ion transport and exploits the capacitive storage benefits of layered silicon.