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.
Highlights
To protect against the reduction of Li metal, protection coating materials or solid electrolytes that are thermodynami-Li metal has been long desired as the anode material with the cally stable or that form stable passivation layers against Li highest theoretical specific capacity and the lowest standard potential to significantly increase the energy density in rechargeable Li-ion battery.[1,2] Enabling Li metal anode has been metal are needed
We considered oxides, sulfides, fluorides, and nitrides, which might be potentially used as solid electrolytes or coating layer materials with Li metal anode
The major discovery of our study is that nitride anion chemistry has significantly better stability against Li metal compared to oxide, sulfide, and halide
Summary
To protect against the reduction of Li metal, protection coating materials or solid electrolytes that are thermodynami-Li metal has been long desired as the anode material with the cally stable or that form stable passivation layers against Li highest theoretical specific capacity and the lowest standard potential to significantly increase the energy density in rechargeable Li-ion battery.[1,2] Enabling Li metal anode has been metal are needed. To protect against the reduction of Li metal, protection coating materials or solid electrolytes that are thermodynami-. Despite that many lithium solid electrolytes were previously. The undesired growth of Li dendrite during cell cycling causes reported to be stable against Li metal, multiple experimental short circuiting in the cell, leading to catastrophic cell failure and first-principles studies confirmed the reduction of solid. Y. Mo Department of Materials Science and Engineering University of Maryland College Park, MD 20742, USA electrolytes, including Li10GeP2S12 (LGPS), NASICON-type Li1.3Al0.3Ti1.7(PO4) (LATP), and perovskite Li0.33La0.56TiO3 (LLTO).[20,21,22,23,24,25,26,27] In these materials, Li metal reduces Ge and Ti cations, forming Li Ge alloy and lithium titanate, respectively. Even for the well-demonstrated Li-compatible LiPON materials, recent computational and in situ experimental
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