Revealing the Multifunctions of Li3N in the Suspension Electrolyte for Lithium Metal Batteries,ACS Nano

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Revealing the Multifunctions of Li3N in the Suspension Electrolyte for Lithium Metal Batteries
ACS Nano ( IF 15.8 ) Pub Date : 2023-01-26 , DOI: 10.1021/acsnano.2c12470
Mun Sek Kim _{1,

2} , Zewen Zhang ₁ , Jingyang Wang _{1,

3} , Solomon T Oyakhire ₂ , Sang Cheol Kim ₁ , Zhiao Yu _{2,

4} , Yuelang Chen _{2,

4} , David T Boyle _{1,

4} , Yusheng Ye ₁ , Zhuojun Huang _{1,

2} , Wenbo Zhang ₁ , Rong Xu ₁ , Philaphon Sayavong _{1,

4} , Stacey F Bent ₂ , Jian Qin ₂ , Zhenan Bao ₂ , Yi Cui _{1,

5,

6}

Affiliation

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, Li₃N is often found in the SEIs of high-performance LMBs. Herein, we elucidate new features of Li₃N 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 Li₃N 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.

中文翻译：

揭示锂金属电池悬浮电解液中 Li3N 的多功能性

锂金属负极上富含无机物的固体电解质界面 (SEI) 可改善锂金属电池 (LMB) 的电化学性能。因此，基本了解基本无机化合物在 SEI 中的作用对于实现和开发高性能 LMB 至关重要。在针对锂金属负极观察到的常见 SEI 无机化合物中，Li ₃ N 经常出现在高性能 LMB 的 SEI 中。在此，我们通过利用有助于改善锂金属负极电化学性能的悬浮电解质设计阐明了 Li ₃ N的新特性。通过实证和计算研究，我们表明 Li ₃^{N 引导 Li 沿其表面电沉积，通过减少 Li +}溶剂配位创造弱溶剂化环境，在 Li 金属负极上诱导有机贫乏的 SEI，并促进 Li ⁺在电解质中的传输。重要的是，认识到 SEI 无机物对锂金属负极的特定作用可以作为通过 LMB 电解质工程设计和优化 SEI 的合理指南之一。

更新日期：2023-01-26

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