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

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.