Enabling Stable and Low‐Strain Lithium Plating/Stripping with 2D Layered Transition Metal Carbides by Forming Li‐Zipped MXenes and a Li Halide‐Rich Solid Electrolyte Interphase

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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 Ti 3 C 2 I 2 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 LiNi 0.8 Mn 0.1 Co 0.1 O 2 and Ti 3 C 2 I 2 @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.