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CPP: Fachverband Chemische Physik und Polymerphysik

CPP 19: Energy Storage and Batteries II

CPP 19.1: Talk

Tuesday, March 19, 2024, 09:30–09:45, H 0111

Reactive molecular dynamics simulations of Lithium-ion battery electrolyte degradation — •Youssef Mabrouk¹, Diddo Diddens², and Andreas Heuer³ — ¹Forschungszentrum Jülich GmbH, Helmholtz-Institute Münster (IEK-12), Corrensstraße 46, 48149 Münster, Germany — ²Forschungszentrum Jülich GmbH, Helmholtz-Institute Münster (IEK-12), Corrensstraße 46, 48149 Münster, Germany — ³Institute of Physical Chemistry, University of Münster, Corrensstrasse 28/30, 48149 Münster, Germany

The development of reliable computational methods for novel battery materials has become essential due to the recently intensified research efforts on more sustainable energy storage materials. Here, we use a recently developed framework allowing to consistently incorporate quantum-mechanical activation barriers to classical molecular dynamics simulations to study the reductive solvent decomposition and formation of the solid electrolyte interphase for a graphite/carbonate electrolyte interface. We focus on deriving condensed-phase effective rates based on the elementary gas-phase reduction and decomposition energy barriers. After a short initial transient limited by the elementary barriers, we observe that the effective rate shows a transition to a kinetically slow regime influenced by the changing coordination environment and the ionic fluxes between the bulk electrolyte and the interface. We also discuss the impact of the decomposition on the ionic mobility. Thus, our work shows how elementary first-principles properties can be mechanistically leveraged to provide fundamental insights into electrochemical stability of battery electrolytes.

Keywords: Lithium-ion battery; Solid-electrolyte interphase formation; First-principles calculations; Molecular dynamics; Density-functional theory