Insights into the Structure and Dynamics of Water at Co₃O₄(001) Using a High-Dimensional Neural Network Potential

2025/08/30 by Amir Omranpour, Jörg Behler, Omranpour, Amir +1 · 1 citation
Energy · Materials Science · Physics and Astronomy · #Advanced Chemical Physics Studies #Chemical Physics (physics.chem-ph) #Electrocatalysts for Energy Conversion #FOS: Physical sciences #Machine Learning in Materials Science #Materials Science (cond-mat.mtrl-sci)

paper · pdf · doi:10.48550/arxiv.2509.00322

openalex publication_date 2025/08/30 · openalex created_date 2025/10/10 · openalex updated_date 2026/07/28

Abstract

Co₃O₄ is an important catalyst for the oxidation of organic molecules in the liquid phase. Still, understanding the atomistic details of Co₃O₄-water interfaces under operando conditions remains extremely challenging. While ab initio molecular dynamics have become an essential tool for investigating these dynamic interfaces in silico, they are limited to only a few picoseconds and a few hundred atoms. In this work, we overcome these limitations by training a high-dimensional neural network potential (HDNNP) on density functional theory data, which allows us to significantly extend the accessible time and length scales. Employing this HDNNP, we perform simulations to unravel the structure, dynamics, and reactivity of Co₃O₄(001)-water interfaces in detail. Our simulations reveal distinct characteristics of the two possible A and B terminations. The B-terminated surface stabilizes a compact, quasi-epitaxial hydration layer with strong templating effects, enhanced hydroxylation, and a well-organized hydrogen-bond network. In contrast, the A-termination forms a more diffuse contact layer with weaker templating, lower hydroxylation, and less ordered interfacial water. Extended simulations further uncover proton transfer pathways, including intermittent protonation of surface hydroxyls, migration of water molecules into the epitaxial layer, and rare hydronium-like configurations.

Citations

• Machine Learning Potentials for Heterogeneous Catalysis
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Cited by

• A Combined Theoretical and Experimental Study of Oxygen Vacancies in Co₃O₄ for Liquid-Phase Oxidation Catalysis

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