Stabilizing Lithium Metal Batteries by Synergistic Effect of High Ionic Transfer Separator and Lithium−Boron Composite Material Anode

The development of lithium (Li) metal batteries (LMBs) has been limited by problems, such as severe dendrite growth, drastic interfacial reactions, and large volume change. Herein, an LMB (8AP@LiB) combining agraphene oxide-poly(ethylene oxide) (PEO) functionalized polypropylene separator (8AP) with a lithium-boron (LiB) anode is designed to overcome these problems. Raman results demonstrate that the PEO chain on 8AP can influence the Li⁺ solvation structure in the electrolyte, resulting in Li⁺ homogeneous diffusion and Li⁺ deposition barrier reduction. 8AP exhibits good ionic conductivity (4.9 × 10^-4 S cm^-1), a high Li⁺ migration number (0.88), and a significant electrolyte uptake (293%). The 3D LiB skeleton can significantly reduce the anode volume changes and local current density during the charging/discharging process. Therefore, 8AP@LiB effectively regulates the Li⁺ flux and promotes the uniform Li deposition without dendrites. The Li||Li symmetrical cells of 8AP@LiB exhibit a high electrochemical stability of up to 1000 h at 1 mA cm^-2 and 5 mAh cm^-2. Importantly, the Li||LiFePO₄ full cells of 8AP@LiB achieve an impressive 2000 cycles at 2C, while maintaining a high-capacity retention of 86%. The synergistic effect of the functionalized separator and LiB anode might provide a direction for the development of high-performance LMBs. © 2023 American Chemical Society.