Towards high performance Li metal batteries: Surface functionalized graphene separator with improved electrochemical kinetics and stability

•Surface functionalization is conducted on the graphene separator.•Enhanced Li-ion diffusivity is achieved by surface functionalized graphene separator.•Moreover, a flexible SEI layer is formed in Li/Cu cell using this separator.•The surface functionalized graphene separator leads to excellent cycle performance. Lithium (Li) metal is a promising anode for next-generation batteries owing to its ultrahigh theoretical capacity (3,860 mAh g−1) and the lowest reduction potential (−3.04 vs SHE at RT). However, the development of Li-metal batteries (LMBs) is still in the research stage due to the inherent problems related to the growth of Li dendrites and unlimited volume change in Li metal. Among diverse approaches, the introduction of functional separators is regarded as an effective strategy for improving the safety and electrochemical performance of LMBs. Herein, we deposited two different graphene layers onto the separators to explore the influence of surface functionalized graphene layer on the electrochemical performance and cycle stability of LMBs. When a surface functionalized graphene separator (SFGS) was used in the LMBs, it exhibited superior electrolyte wettability than a graphene separator (GS), contributing to the improved ionic conductivity and homogeneous Li-ion flux. Due to the improved electrochemical kinetics and reversible electrochemical reactions, Li/Cu cells with the SFGS exhibited the most stable cycle performance with a high Coulombic efficiency of 98 % over 200 cycles compared with other Li/Cu cells. Our strategy would resolve many issues related to the poor electrochemical reversibility of Li-metal anodes and advance the development of practical surface-modified separators for high-performance LMBs.