An In-Situ Raman Spectroscopic Study on the Interfacial Process of Carbonate-Based Electrolyte on Nanostructured Silver Electrode

Authors

Yu Gu, State Key Laboratory of Physical Chemistry of Solid Surfaces, Innovation Laboratory for Sciences and Technologies of Energy Materials of Fujian Province (IKKEM), College of Chemistry and Chemical Engineering, Xiamen University, Xiamen 361005, Fujian, ChinaFollow
Yuan-Fei Hu, State Key Laboratory of Physical Chemistry of Solid Surfaces, Innovation Laboratory for Sciences and Technologies of Energy Materials of Fujian Province (IKKEM), College of Chemistry and Chemical Engineering, Xiamen University, Xiamen 361005, Fujian, China
Wei-Wei Wang, State Key Laboratory of Physical Chemistry of Solid Surfaces, Innovation Laboratory for Sciences and Technologies of Energy Materials of Fujian Province (IKKEM), College of Chemistry and Chemical Engineering, Xiamen University, Xiamen 361005, Fujian, China
En-Ming You, State Key Laboratory of Physical Chemistry of Solid Surfaces, Innovation Laboratory for Sciences and Technologies of Energy Materials of Fujian Province (IKKEM), College of Chemistry and Chemical Engineering, Xiamen University, Xiamen 361005, Fujian, China
Shuai Tang, State Key Laboratory of Physical Chemistry of Solid Surfaces, Innovation Laboratory for Sciences and Technologies of Energy Materials of Fujian Province (IKKEM), College of Chemistry and Chemical Engineering, Xiamen University, Xiamen 361005, Fujian, China; College of Chemistry, Zhengzhou University, Zhengzhou 450001, Fujian, China
Jian-Jia Su, State Key Laboratory of Physical Chemistry of Solid Surfaces, Innovation Laboratory for Sciences and Technologies of Energy Materials of Fujian Province (IKKEM), College of Chemistry and Chemical Engineering, Xiamen University, Xiamen 361005, Fujian, China
Jun Yi, State Key Laboratory of Physical Chemistry of Solid Surfaces, Innovation Laboratory for Sciences and Technologies of Energy Materials of Fujian Province (IKKEM), College of Chemistry and Chemical Engineering, Xiamen University, Xiamen 361005, Fujian, China
Jia-Wei Yan, State Key Laboratory of Physical Chemistry of Solid Surfaces, Innovation Laboratory for Sciences and Technologies of Energy Materials of Fujian Province (IKKEM), College of Chemistry and Chemical Engineering, Xiamen University, Xiamen 361005, Fujian, China
Zhong-Qun Tian, State Key Laboratory of Physical Chemistry of Solid Surfaces, Innovation Laboratory for Sciences and Technologies of Energy Materials of Fujian Province (IKKEM), College of Chemistry and Chemical Engineering, Xiamen University, Xiamen 361005, Fujian, China
Bing-Wei Mao, State Key Laboratory of Physical Chemistry of Solid Surfaces, Innovation Laboratory for Sciences and Technologies of Energy Materials of Fujian Province (IKKEM), College of Chemistry and Chemical Engineering, Xiamen University, Xiamen 361005, Fujian, ChinaFollow

Corresponding Author

Yu Gu(ygu@xmu.edu.cn);
Bing-Wei Mao (bwmao@xmu.edu.cn)

Abstract

The solid-electrolyte interphase (SEI) plays a key role in anodes for rechargeable lithium-based battery technologies. However, a thorough understanding in the mechanisms of SEI formation and evolution remains a major challenge, 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 subsequent 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.

Graphical Abstract

Keywords

solid-electrolyte interphase; in-situ SERS; anodes; lithium-based batteries

DOI Link

https://doi.org/10.13208/j.electrochem.2301261

Creative Commons License

This work is licensed under a Creative Commons Attribution 4.0 International License.

Publication Date

2023-12-28

Online Available Date

2023-09-19

Revised Date

2023-03-03

Received Date

2023-01-26

Recommended Citation

Yu Gu, Yuan-Fei Hu, Wei-Wei Wang, En-Ming You, Shuai Tang, Jian-Jia Su, Jun Yi, Jia-Wei Yan, Zhong-Qun Tian, Bing-Wei Mao. An In-Situ Raman Spectroscopic Study on the Interfacial Process of Carbonate-Based Electrolyte on Nanostructured Silver Electrode[J]. Journal of Electrochemistry, 2023 , 29(12): 2301261.
DOI: 10.13208/j.electrochem.2301261
Available at: https://jelectrochem.xmu.edu.cn/journal/vol29/iss12/2