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DOE OSTI · 2203080

Modeling the aqueous interface of amorphous TiO 2 using deep potential molecular dynamics

Ding, Zhutian·Selloni, Annabella
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Abstract

Amorphous titanium dioxide (a-TiO 2 ) 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-TiO 2 surface and aqueous interface, particularly at the microscopic level. In this work, we construct a model of the a-TiO 2 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-TiO 2 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-TiO 2 surface lacks distinct layers normally found at the aqueous interface of crystalline TiO 2 , leading to an ~10 times faster diffusion of water at the interface. Bridging hydroxyls (Ti 2 –O b H) resulting from water dissociation decay several times more slowly than terminal hydroxyls (Ti–O w H) due to fast Ti–O w H 2 → Ti–O w H proton exchange events. These results provide a basis for a detailed understanding of the properties of a-TiO 2 in electrochemical environments. Moreover, the procedure of generating the a-TiO 2 -interface employed here is generally applicable to studying the aqueous interfaces of amorphous metal oxides.

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37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRYAqueous interfacesArtificial neural networksDensity functional theoryMolecular dynamics

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Ding, Zhutian, Selloni, Annabella. 2023-07-10. Modeling the aqueous interface of amorphous TiO 2 using deep potential molecular dynamics. https://doi.org/10.1063/5.0157188

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