Uniformizing the lithium deposition by gradient lithiophilicity and conductivity for stable lithium-metal batteries

The practical application of lithium metal batteries is hindered by the poor reversibility and large volume change caused by the uncontrollable dendritic growth and the highly reactive surface. In this work, favorable Li deposition is achieved by generating gradient lithiophilicity and conductivity in an Ag-decorated graphene/holey graphene film (G-HGA). Dendrite-free Li metal is deposited on the G-HGA matrix, which greatly reduces the surface area and suppresses the side reaction between the electrolyte and the dendritic Li. The average Li-metal plating-stripping coulombic efficiency (CE) on the G-HGA matrix maintains ∼98.7% over 350 cycles, compared to a worse average CE (∼97.3%) with the bare Cu matrix, only for less than 100 cycles. A full cell constructed by using LiFePO₄ and prelithiated G-HGA exhibits excellent rate capability and a high capacity retention of 99.6% for 175 cycles at a low negative to positive capacity ratio of 1.13. This advanced design can inspire further development of high-energy and long-lived Li-metal batteries.