Abstract

Two-dimensional (2D) layered materials demonstrate prominent advantage in regulating lithium plating/stripping behavior by confining lithium diffusion/plating within interlayer gaps. However, achieving effective interlayer confined lithium diffusion/plating without compromising the stability of bulk-structural and the solid electrolyte interphase (SEI) remains a considerable challenge. This paper presents an electrochemical scissor and lithium zipper-driven protocol for realizing interlayer confined lithium plating with pretty-low strain and volume change. In this protocol, lithium serves as a "zipper" to reunite the adjacent MXene back to MAX-like phase to markedly enhance the structural stability, and a lithium halide-rich SEI is formed by electrochemically removing the terminals of halogenated MXenes to maintain the stability and rapid lithium ions diffusion of SEI. When the Ti3 C2 I2 serves as the host for lithium plating, the average coulomb efficiency exceeds 97.0 % after 320 lithium plating/stripping cycles in conventional ester electrolyte. Furthermore, a full cell comprising of LiNi0.8 Mn0.1 Co0.1 O2 and Ti3 C2 I2 @Li exhibits a capacity retention rate of 73.4 % after 200 cycles even under high cathode mass-loading (20 mg cm-2 ) and a low negative/positive capacity ratio of 1.4. Our findings advance the understanding of interlayer confined lithium plating in 2D layered materials and provide a new direction in regulating lithium and other metal plating/stripping behaviors.

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