Insights into lithium manganese oxide-water interfaces using machine learning potentials

Abstract

Unraveling the atomistic and the electronic structure of solid-liquid interfaces is the key to the design of new materials for many important applications, from heterogeneous catalysis to battery technology. Density functional theory (DFT) calculations can in principle provide a reliable description of such interfaces, but the high computational costs severely restrict the accessible time and length scales. Here, we report machine learning-driven simulations of various interfaces between water and lithium manganese oxide (Li${}_x$Mn${}_2$O${}_4$), an important electrode material in lithium ion batteries and a catalyst for the oxygen evolution reaction. We employ a high-dimensional neural network potential (HDNNP) to compute the energies and forces several orders of magnitude faster than DFT without loss in accuracy. In addition, a high-dimensional neural network for spin prediction (HDNNS) is utilized to analyze the electronic structure of the manganese ions. Combining these methods, a series of interfaces is investigated by large-scale molecular dynamics. The simulations allow us to gain insights into a variety of properties like the dissociation of water molecules, proton transfer processes, and hydrogen bonds, as well as the geometric and electronic structure of the solid surfaces including the manganese oxidation state distribution, Jahn-Teller distortions, and electron hopping.

21 pages, 13 figures

References in corpus (10)

• Machine learning for molecular simulation
• Machine Learning Unifies the Modelling of Materials and Molecules
• How van der Waals interactions determine the unique properties of water
• Ab initio theory and modeling of water
• Electronic Structure Modeling of Electrochemical Reactions at Electrode/Electrolyte Interfaces in Lithium Ion Batteries
• First Principles Modeling of the Initial Stages of Organic Solvent Decomposition on Li(x)Mn(2)O(4) (100) Surfaces
• First Principles Modeling of Mn(II) Migration above and Dissolution from Li(x)Mn(2)O(4) (001) Surfaces
• Solvent Induced Proton Hopping at a Water-Oxide Interface
• Decisive role of nuclear quantum effects on surface mediated water dissociation at finite temperature
• A criticial view on e${}_g$ occupancy as a descriptor for oxygen evolution catalytic activity in LiMn${}_2$O${}_4$ nanoparticles

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