Mechanism of Fe(II) Chemisorption on Hematite(001) Revealed by Reactive Neural Network Potential Molecular Dynamics

Joll, Kit; Schienbein, Philipp; Rosso, Kevin M.; Blumberger, Jochen

doi:10.1021/acs.jpclett.4c03252

Title: Mechanism of Fe(II) Chemisorption on Hematite(001) Revealed by Reactive Neural Network Potential Molecular Dynamics

Journal Article · 16 January 2025 · Journal of Physical Chemistry Letters

DOI: https://doi.org/10.1021/acs.jpclett.4c03252 · OSTI ID:2500913

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Univ. College London (United Kingdom)
Univ. College London (United Kingdom); Ruhr Univ., Bochum (Germany); Research Alliance Ruhr, Bochum (Germany)
Pacific Northwest National Laboratory (PNNL), Richland, WA (United States)

Atomic-scale understanding of important geochemical processes including sorption, dissolution, nucleation, and crystal growth is difficult to obtain from experimental measurements alone and would benefit from strong continuous progress in molecular simulation. To this end, we present a reactive neural network potential-based molecular dynamics approach to simulate the interaction of aqueous ions on mineral surfaces in contact with liquid water, taking Fe(II) on hematite(001) as a model system. We show that a single neural network potential predicts rate constants for water exchange for aqueous Fe(II) and for the exergonic chemisorption of aqueous Fe(II) on hematite(001) in good agreement with experimental observations. The neural network potential developed herein allows one to converge free energy profiles and transmission coefficients at density functional theory-level accuracy outperforming state-of-the-art classical force field potentials. This suggests that machine learning potential molecular dynamics should become the method of choice for atomistic studies of geochemical processes.

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Research Organization:: Pacific Northwest National Laboratory (PNNL), Richland, WA (United States)

Sponsoring Organization:: USDOE; USDOE Office of Science (SC), Basic Energy Sciences (BES). Chemical Sciences, Geosciences & Biosciences Division (CSGB)

Grant/Contract Number:: AC05-76RL01830

OSTI ID:: 2500913

Report Number(s):: PNNL-SA--207725

Journal Information:: Journal of Physical Chemistry Letters, Journal Name: Journal of Physical Chemistry Letters Journal Issue: 4 Vol. 16; ISSN 1948-7185

Publisher:: American Chemical SocietyCopyright Statement

Country of Publication:: United States

Language:: English

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