Enabling accurate modelling of materials for a solid electrolyte interphase in lithium-ion batteries using effective machine learning interatomic potentials

Abstract

Accurate modelling of the structural and dynamic properties of the solid electrolyte interphase (SEI) in lithium-ion batteries remains a longstanding challenge due to the high complexity of the SEI structure and the lack of structural information. Atomistic simulations using molecular dynamics (MD) can provide insights into the structure of the SEI but require large models and accurate interatomic potentials; however, existing computational tools struggle to evaluate these potentials in mixed-material systems efficiently and reliably. Here, we demonstrate the effectiveness of machine learning interatomic potentials (MLIPs) defined using amorphous structures as reference data, specifically the moment tensor potential (MTP), combined with density functional theory (DFT) calculations and active learning loops that enable rapid sampling of MD trajectories. For SEI relevant materials (e.g., Li₂CO₃, bulk Li, LiPF₆, and Li₂EDC), our trained MTP models accurately capture the key structural properties (e.g., lattice parameters, elastic constants, or phonon spectra). For the dynamical properties of monoclinic Li₂CO₃ and amorphous Li₂EDC, the models are validated against previous theoretical predictions in the literature. Particularly, we illustrate the finite temperature effects on computing energy barriers. The determined mechanism of dominant diffusion carriers (Li vacancy, interstitial Li, and Li Frenkel pair) in Li₂CO₃ is highly consistent with DFT calculations. Furthermore, we show that the generated training datasets can be applied to train graph-neural-network (GNN)-based interatomic potentials that can further improve accuracy. The developed machine learning workflow provides a scalable approach for SEI modelling, enabling simulations at larger time and length scales to tackle the limitations of conventional DFT methods.