Stable lithium anode enabled by biphasic hybrid SEI layer toward high-performance lithium metal batteries

The Li/Li symmetric cell with SbF3-modified Li as electrodes can achieve stable cycling over 400h at high current density of 3.0 mA cm−2 for fixed areal capacity of 3.0 mAh cm−2 and realize dendrite-free surface state. [Display omitted] •An artificial Li3Sb/LiF biphasic hybrid SEI layer was successfully constructed.•This biphasic hybrid SEI layer can effectively regulate Li ion depositing behavior.•The Li/Li symmetric cells with SF-Li anodes exhibit extended cycling lifespan.•The LMBs with SF-Li anodes deliver superior cycling performance and high CE. Lithium (Li) metal has been proposed as the most promising anode for secondary lithium batteries with high energy density due to its considerable theoretical capacity (3860 mAh g−1) and lowest electrochemical potential (-3.04 V vs standard hydrogen electrode). However, the uncontrollable dendrite Li issues over repeated plating/stripping process results in huge volume change, low Coulombic efficiencies (CEs), and poor cycling performance. Here, a solid electrolyte interphase (SEI) layer mainly consisting of biphasic hybrid Li3Sb and LiF has been successfully in situ constructed on Li surface by spontaneous chemical reaction between Li and SbF3. The modified SEI can induce Li ions depositing on the linked-particle layer resulting from the relative low lithium diffusion coefficient of SEI layer component. The Li/Li symmetric cells with SbF3-modified Li (SF-Li) anodes show stable cycling over 400 h at 3.0 mA cm−2 for 3.0 mAh cm−2. The Li-S batteries with SF-Li anodes and ether-based electrolyte can achieve steady long-term cycling performance and high CEs. Particularly, the high voltage LiCoO2 (LCO)/Li batteries with SF-Li anodes and carbonate-based electrolyte also deliver excellent electrochemical properties even at harsh conditions. This work offers a new strategy to regulate Li ion deposition and benefits for the further development of safe Li metal batteries (LMBs).