Modeling the aqueous interface of amorphous TiO2 using deep potential molecular dynamics

Ding, Zhutian; Selloni, Annabella

doi:10.1063/5.0157188

Modeling the aqueous interface of amorphous TiO₂ using deep potential molecular dynamics

Journal Article · Mon Jul 10 00:00:00 EDT 2023 · Journal of Chemical Physics

DOI:https://doi.org/10.1063/5.0157188· OSTI ID:2203080

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Princeton University, NJ (United States); Princeton University
Princeton University, NJ (United States)

Amorphous titanium dioxide (a-TiO₂) is widely used as a coating material in applications such as electrochemistry and self-cleaning surfaces where its interface with water has a central role. However, little is known about the structures of the a-TiO₂ surface and aqueous interface, particularly at the microscopic level. In this work, we construct a model of the a-TiO₂ surface via a cut-melt-and-quench procedure based on molecular dynamics simulations with deep neural network potentials (DPs) trained on density functional theory data. After interfacing the a-TiO₂ surface with water, we investigate the structure and dynamics of the resulting system using a combination of DP-based molecular dynamics (DPMD) and ab initio molecular dynamics (AIMD) simulations. Both AIMD and DPMD simulations reveal that the distribution of water on the a-TiO₂ surface lacks distinct layers normally found at the aqueous interface of crystalline TiO₂, leading to an ~10 times faster diffusion of water at the interface. Bridging hydroxyls (Ti₂–O_bH) resulting from water dissociation decay several times more slowly than terminal hydroxyls (Ti–O_wH) due to fast Ti–O_wH₂ → Ti–O_wH proton exchange events. These results provide a basis for a detailed understanding of the properties of a-TiO₂ in electrochemical environments. Moreover, the procedure of generating the a-TiO₂-interface employed here is generally applicable to studying the aqueous interfaces of amorphous metal oxides.

View Accepted Manuscript (DOE)

Research Organization:: Princeton University, NJ (United States)

Sponsoring Organization:: USDOE Office of Science (SC), Basic Energy Sciences (BES)

Grant/Contract Number:: AC02-05CH11231; SC0007347; SC0019394

OSTI ID:: 2203080

Journal Information:: Journal of Chemical Physics, Journal Name: Journal of Chemical Physics Journal Issue: 2 Vol. 159; ISSN 0021-9606

Publisher:: American Institute of Physics (AIP)Copyright Statement

Country of Publication:: United States

Language:: English

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Modeling the aqueous interface of amorphous TiO2 using deep potential molecular dynamics

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Modeling the aqueous interface of amorphous TiO₂ using deep potential molecular dynamics