By introducing Li insufficiency, we interestingly found that m-LiBC exhibits a higher capacity (220 mA h g) than the original o-LiBC (50 mA h g). This improved capacity benefits from its structural evolution, with the interlayer rearrangement changed from "ABABAB" (o-LiBC) to "ABAABA" (m-LiBC) stacking, triggered by Li insufficiency. This understanding of interlayer rearrangement for LiBC may open a new avenue to activate Li extraction in other lithium compounds.
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