Abstract
Lithium metal battery is a promising candidate for high-energy-density energy storage. Unfortunately, the strongly reducing nature of lithium metal has been an outstanding challenge causing poor stability and low coulombic efficiency in lithium batteries. For decades, there are significant research efforts to stabilize lithium metal anode. However, such efforts are greatly impeded by the lack of knowledge about lithium-stable materials chemistry. So far, only a few materials are known to be stable against Li metal. To resolve this outstanding challenge, lithium-stable materials have been uncovered out of chemistry across the periodic table using first-principles calculations based on large materials database. It is found that most oxides, sulfides, and halides, commonly studied as protection materials, are reduced by lithium metal due to the reduction of metal cations. It is discovered that nitride anion chemistry exhibits unique stability against Li metal, which is either thermodynamically intrinsic or a result of stable passivation. The results here establish essential guidelines for selecting, designing, and discovering materials for lithium metal protection, and propose multiple novel strategies of using nitride materials and high nitrogen doping to form stable solid-electrolyte-interphase for lithium metal anode, paving the way for high-energy rechargeable lithium batteries.