电化学（中英文）2023，Vol.29Issue(12)：12-23,12.DOI:10.13208/j.electrochem.2301261
碳酸酯类电解液中纳米银电极界面过程的原位拉曼光谱研究
An In-Situ Raman Spectroscopic Study on the Interfacial Process of Carbonate-Based Electrolyte on Nanostructured Silver Electrode
摘要
Abstract
The solid-electrolyte interphase(SEI)plays a key role in anodes for rechargeable lithium-based battery technolo-gies.However,a thorough understanding in the mechanisms of SEI formation and evolution remains a major chal-lenge,hindering the rapid development and wide applications of Li-based batteries.Here,we devise a borrowing surface-enhanced Raman scattering(SERS)activity strategy by utilizing a size optimized Ag nanosubstrate to in-situ monitor the formation and evolution of SEI,as well as its structure and chemistry in an ethylene carbonate-based electrolyte.To ensure a reliable in-situ SERS investigation,we designed a strict air-tight Raman cell with a three-electrode configuration.Based on the potential-dependent spectroscopic information,we revealed that the SEI formed in an EC-based electrolyte presents a double-layer structure,comprising a thin inorganic inner layer and an organic-rich outer layer.We also identified that LEMC,rather than LEDC,is the major component of EC reduction,and the critical role of metallic Li in the formation of stable SEI is preliminary explored.Nevertheless,identifying the SEI compositions is only feasible before Li deposition on the Ag surface.After the formation of Li-Ag alloys,the subse-quent evolution of SEI could not be detected due to the change in the dielectric constant of Ag after the lithiation.Our work provides a real-time spectroscopic method for investigating interfacial processes of anodes,which is beneficial to the understanding of SEI formation and evolution and thus provides guidance for the development of rationally designed SEI in Li-based batteries.关键词
固态电解质界面相/原位SERS/负极界面/锂电池Key words
Solid-electrolyte interphase/In-situ SERS/Anodes/Lithium-based batteries引用本文复制引用
谷宇,毛秉伟,胡元飞,王卫伟,尤恩铭,唐帅,苏建加,易骏,颜佳伟,田中群..碳酸酯类电解液中纳米银电极界面过程的原位拉曼光谱研究[J].电化学（中英文）,2023,29(12):12-23,12.基金项目
This work was supported by the National Natu-ral Science Foundation of China(No.22002129,No.21972119,No.21991151,No.22202162,No.22102137,No.22072123),and the China Post-doctoral Science Foundation(No.2019TQ0177,No.2022T150548,No.2022M722648).The authors wish to thank Professors Bin Ren and Zhi-Cong Zeng for their assistances in providing helpful discussion and valuable comments on the manuscript. （No.22002129,No.21972119,No.21991151,No.22202162,No.22102137,No.22072123）
