Regensburg 2025 – scientific programme
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O: Fachverband Oberflächenphysik
O 34: Poster Solid-Liquid Interfaces: Reactions and Electrochemistry
O 34.1: Poster
Tuesday, March 18, 2025, 13:30–15:30, P3
Free Energy Calculations of Electrolyte Decomposition Reactions on Lithium Battery Electrodes — •Azad Kirsan and Bernd Meyer — Interdisciplinary Center for Molecular Materials and Computer Chemistry Center, FAU Erlangen-Nürnberg
For the development of lithium metal batteries (LMBs) it is essential to understand how a stable solid electrolyte interphase (SEI) is formed. Ethylene carbonate (EC), a commonly used electrolyte, plays a critical role in SEI formation through its electrochemical decomposition at the electrode surface. Thus, insights into the mechanism of the decomposition reaction are of crucial importance for understanding the processes that govern SEI composition, structure and stability.
In this work, ab initio molecular dynamics simulations using state-of-the-art enhanced sampling methods (metadynamics, umbrella sampling, well-sliced metadynamics [1]) including explicitly the liquid electrolyte were performed in order to unravel the reaction mechanisms of the first steps of the EC dissociation on a Li2O surface. The trajectories, encompassing more than 1 ns of sampling time, were used to reconstruct the free energy surfaces and obtain activation barriers for the decomposition reaction.
[1] S. Awasthi, V. Kapil, N.N. Nair, J. Comput. Chem. 37 (2016) 1413
Keywords: lithium metal batteries; electrolyte decomposition; molecular dynamics; free energy sampling