Department of Materials Science and Engineering, Stanford University, Stanford, California 94305, United States.
Department of Chemical Engineering, Stanford University, Stanford, California 94305, United States.
ACS Nano. 2023 Feb 14;17(3):3168-3180. doi: 10.1021/acsnano.2c12470. Epub 2023 Jan 26.
Inorganic-rich solid-electrolyte interphases (SEIs) on Li metal anodes improve the electrochemical performance of Li metal batteries (LMBs). Therefore, a fundamental understanding of the roles played by essential inorganic compounds in SEIs is critical to realizing and developing high-performance LMBs. Among the prevalent SEI inorganic compounds observed for Li metal anodes, LiN is often found in the SEIs of high-performance LMBs. Herein, we elucidate new features of LiN by utilizing a suspension electrolyte design that contributes to the improved electrochemical performance of the Li metal anode. Through empirical and computational studies, we show that LiN guides Li electrodeposition along its surface, creates a weakly solvating environment by decreasing Li-solvent coordination, induces organic-poor SEI on the Li metal anode, and facilitates Li transport in the electrolyte. Importantly, recognizing specific roles of SEI inorganics for Li metal anodes can serve as one of the rational guidelines to design and optimize SEIs through electrolyte engineering for LMBs.
富含无机物的固体电解质界面(SEI)可以改善锂金属电池(LMB)的电化学性能。因此,深入了解 SEI 中基本无机化合物的作用对于实现和开发高性能 LMB 至关重要。在观察到的用于锂金属负极的 SEI 中,LiN 通常存在于高性能 LMB 的 SEI 中。在此,我们通过利用悬浮电解质设计阐明了 LiN 的新特征,该设计有助于提高锂金属负极的电化学性能。通过经验和计算研究,我们表明 LiN 引导 Li 沿其表面沉积,通过减少 Li-溶剂配位来创建一种弱溶剂化环境,在锂金属阳极上诱导出贫有机 SEI,并促进电解质中的 Li 传输。重要的是,认识到 SEI 无机物对于锂金属阳极的特定作用可以作为通过电解质工程来设计和优化 LMB 中 SEI 的合理指导之一。