Resolving nanostructure and chemistry of solid-electrolyte interphase on lithium anodes by depth-sensitive plasmon-enhanced Raman spectroscopy

Yu Gu, En-Ming You, Jian- De Lin, Jun-Hao Wang, Si-Heng Luo, Ru-Yu Zhou, Chen-Jie Zhang, Jian-Lin Yao, Hui-Yang Li, Gen Li, Wei-Wei Wang, Yu Qiao, Jia-Wei Yan, Wu De-Yin, Guo-Kun Liu, Li Zhang, Jian-Feng Li, Rong Xu, Zhong-Qun Tian (), Yi Cui () and Bing-Wei Mao ()
Additional contact information
Yu Gu: Xiamen University
En-Ming You: Xiamen University
Jian- De Lin: Xiamen University
Jun-Hao Wang: Xiamen University
Si-Heng Luo: Xiamen University
Ru-Yu Zhou: Xiamen University
Chen-Jie Zhang: Soochow University
Jian-Lin Yao: Soochow University
Hui-Yang Li: Xiamen University
Gen Li: Xiamen University
Wei-Wei Wang: Xiamen University
Yu Qiao: Xiamen University
Jia-Wei Yan: Xiamen University
Wu De-Yin: Xiamen University
Guo-Kun Liu: Xiamen University
Li Zhang: Xiamen University
Jian-Feng Li: Xiamen University
Rong Xu: Stanford University
Zhong-Qun Tian: Xiamen University
Yi Cui: Stanford University
Bing-Wei Mao: Xiamen University

Nature Communications, 2023, vol. 14, issue 1, 1-11

Abstract: Abstract The solid-electrolyte interphase (SEI) plays crucial roles for the reversible operation of lithium metal batteries. However, fundamental understanding of the mechanisms of SEI formation and evolution is still limited. Herein, we develop a depth-sensitive plasmon-enhanced Raman spectroscopy (DS-PERS) method to enable in-situ and nondestructive characterization of the nanostructure and chemistry of SEI, based on synergistic enhancements of localized surface plasmons from nanostructured Cu, shell-isolated Au nanoparticles and Li deposits at different depths. We monitor the sequential formation of SEI in both ether-based and carbonate-based dual-salt electrolytes on a Cu current collector and then on freshly deposited Li, with dramatic chemical reconstruction. The molecular-level insights from the DS-PERS study unravel the profound influences of Li in modifying SEI formation and in turn the roles of SEI in regulating the Li-ion desolvation and the subsequent Li deposition at SEI-coupled interfaces. Last, we develop a cycling protocol that promotes a favorable direct SEI formation route, which significantly enhances the performance of anode-free Li metal batteries.

Date: 2023
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DOI: 10.1038/s41467-023-39192-z

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