Gao, Jingqi;
He, Ruitian;
Wu, Peng;
Luo, Kai H;
(2025)
Unravelling multi-layered structure of native SEI on lithium metal electrode and various electrolytes using reactive molecular dynamics.
Journal of Energy Storage
, 106
, Article 114919. 10.1016/j.est.2024.114919.
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Abstract
Lithium metal batteries, directly utilizing lithium metal as an anode, are promising as new-generation energy storage devices, and the characteristics of the solid electrolyte interphase (SEI) layer are critical to battery operation. However, the roles of electrolyte compositions on the structure and thickness of the passivating SEI film at the atomistic level have been previously overlooked, resulting in poor understanding of SEI characteristics. In this study, the formation of the native SEI layer on lithium metal electrode and various electrolyte composition is scrutinised using ReaxFF molecular dynamics (MD) simulations. The study successfully identifies different layers of the SEI film using charge distribution as a tool. The decrease in lithium density and the increase in the charge states of oxidised lithium atoms contribute to the identification of an inner layer and a transition layer within the previously known interface layer, as well as the sparse layer. Additionally, different reaction schemes are observed through the analysis of ratio between consumed lithium atoms and electrolyte molecules. Furthermore, results show the lithium salt concentration effects in suppressing the growth of the SEI between the lithium anode and the liquid electrolyte, and inhibiting the formation of key SEI components. This work provides new insights into the nature of SEI surface chemistry and potentially facilitates the design of artificial SEI layers and optimal electrolyte solutions.
| Type: | Article |
|---|---|
| Title: | Unravelling multi-layered structure of native SEI on lithium metal electrode and various electrolytes using reactive molecular dynamics |
| Open access status: | An open access version is available from UCL Discovery |
| DOI: | 10.1016/j.est.2024.114919 |
| Publisher version: | https://doi.org/10.1016/j.est.2024.114919 |
| Language: | English |
| Additional information: | © 2024 The Authors. Published by Elsevier Ltd. This is an open access article under the CC BY license (http://creativecommons.org/licenses/by/4.0/). |
| Keywords: | Solid electrolyte interphase, Lithium battery, Molecular dynamics, Reactive force field, Lithium metal electrode |
| UCL classification: | UCL UCL > Provost and Vice Provost Offices > UCL BEAMS UCL > Provost and Vice Provost Offices > UCL BEAMS > Faculty of Engineering Science > Dept of Mechanical Engineering |
| URI: | https://discovery.ucl.ac.uk/id/eprint/10201488 |
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