Visualizing and Regulating Dynamic Evolution of Interfacial Electrolyte Configuration during De-solvation Process on
Junhao Wang1, Jing Luo2, Haichuan Wu1
1State Key Laboratory of Physical Chemistry of Solid Surfaces, Collaborative Innovation Center of Chemistry for Energy Materials (iChEM), Department of Chemistry, College of Chemistry and Chemical Engineering, Xiamen University, 361005, Xiamen, P. R. China.
Angewandte Chemie (International Ed. in English)
|March 5, 2024
Summary
This study reveals how electrolyte configuration impacts solid-electrolyte interphase (SEI) formation on lithium-metal anodes. A novel pulse protocol enhances SEI stability and lithium plating reversibility by restoring interfacial anion concentration.
Area of Science:
- Materials Science
- Electrochemistry
- Battery Technology
Background:
- The solid-electrolyte interphase (SEI) is critical for lithium-metal anode stability.
- SEI formation involves electrolyte decomposition during lithium plating.
- Current strategies often overlook the dynamic electrolyte evolution at the Li/electrolyte interface.
Purpose of the Study:
- To visualize the dynamic changes in Li+-solvent/anion solvation environments at the Li/electrolyte interface.
- To understand how electrolyte configuration influences SEI architecture.
- To develop a strategy for improving SEI formation and lithium-metal battery performance.
Main Methods:
- Electrochemical in situ Fourier-transform infrared (FT-IR) spectroscopy.
- Magnetic resonance imaging (MRI) techniques.
- Pulse plating protocol for electrolyte regulation.
Main Results:
- Synchronous observation of weakened Li+-solvent interaction and an anion-lean interfacial electrolyte.
- Difficulty in forming anion-derived SEI due to the observed electrolyte configuration.
- A pulse protocol effectively restored interfacial anion concentration.
- Fabrication of a LiF-rich SEI layer and improved Li-metal plating/stripping reversibility.
Conclusions:
- The dynamic evolution of the interfacial electrolyte configuration is crucial for SEI formation.
- Electrolyte engineering must account for these dynamic interfacial processes.
- The pulse protocol offers a viable strategy for enhancing lithium-metal anode stability and performance.
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