Polymer–inorganic solid–electrolyte interphase for stable lithium metal batteries under lean electrolyte conditions

The solid–electrolyte interphase (SEI) is pivotal in stabilizing lithium metal anodes for rechargeable batteries. However, the SEI is constantly reforming and consuming electrolyte with cycling. The rational design of a stable SEI is plagued by the failure to control its structure and stability. Here we report a molecular-level SEI design using a reactive polymer composite, which effectively suppresses electrolyte consumption in the formation and maintenance of the SEI. The SEI layer consists of a polymeric lithium salt, lithium fluoride nanoparticles and graphene oxide sheets, as evidenced by cryo-transmission electron microscopy, atomic force microscopy and surface-sensitive spectroscopies. This structure is different from that of a conventional electrolyte-derived SEI and has excellent passivation properties, homogeneity and mechanical strength. The use of the polymer–inorganic SEI enables high-efficiency Li deposition and stable cycling of 4 V Li|LiNi 0.5 Co 0.2 Mn 0.3 O 2 cells under lean electrolyte, limited Li excess and high capacity conditions. The same approach was also applied to design stable SEI layers for sodium and zinc anodes. Solid–electrolyte interphase is crucial for stabilizing lithium metal anodes for rechargeable batteries. A molecular-level design using a reactive polymer composite is now shown to effectively construct a stable SEI layer and suppress electrolyte consumption upon cycling.