Laser‐Induced Solid‐Phase Strategy to Synthesize Single‐Atomic Lithiophilic Sites Enabled Dendrite‐Free Lithium Deposition on Graphene Matrix

Abstract The introduction of metal Single‐atom (SA) to construct lithium‐philic active sites shows the ability to guide uniform lithium deposition and improve the stability of lithium hosts. Nevertheless, the development of facile and expedient methods for synthesizing SA remains a considerable challenge. Herein, The SA metal loaded on graphene (Bi@LrGO) is designed by laser‐induced solid‐phase strategy. The bismuth salts simultaneously decompose under the high local temperature and in the reductive atmosphere induced by laser to form SA metal. Simultaneously, graphene oxide (GO) nanosheets absorb photon energy to be reduced/graphitized into graphene, which serves as anchoring sites for Bismuth Sing‐atom (Bi SA) immobilization. The SA metals, supported on the graphene not only provide sufficient lithiophilic sites but also significantly increase the adsorption energy (−2.11 eV) with lithium atoms, promote the uniform nucleation and deposition of lithium, and inhibit the growth of lithium dendrites. Additionally, the layered structure of the graphene film adapts to the volume change during the repeated lithium plating/stripping process. Therefore, the symmetrical battery‐based Li deposited on Bi@LrGO (Bi@LrGO@Li) achieves an ultra‐long stable cycle life of ≈2400 h at 1 mA cm −2 . In particular, a full cell with LiFePO 4 cathode provides a good capacity retention of 81.2% at 4 C after 600 cycles.