Reversible Deposition of Lithium Particles Enabled by Ultraconformal and Stretchable Graphene Film for Lithium Metal Batteries

Abstract Originating from inhomogeneous Li deposition and dissolution, the formation of dendritic and/or dead Li lies as a fundamental barrier to the practical implementation of Li metal anodes for high‐energy Li‐ion batteries. Here, an ultraconformal and stretchable solid‐electrolyte interphase (SEI) composed of parallelly stacked few‐layer defect‐free graphene nanosheets, which can deform to remain ultraconformal during the expansion and shrinkage of micro‐sized Li metal particles is reported. The shape‐adaptive graphene protective skin is prepared via a facile mechanical method followed by Li stripping, which enables fast Li‐ion diffusion, and inhibits Li dendrites and Li pulverization. The interlayer slips and wrinkles of the graphene film endow the robust protective skin with high stretchability. This work represents a unique strategy of building ultraconformal and stretchable 2D‐materials‐based protective skins on the surface of Li metal toward high‐energy, long‐life, and safe Li metal batteries.