离解(化学)
金红石
锐钛矿
化学物理
水溶液
水的自电离
从头算
材料科学
从头算量子化学方法
光催化
吸附
化学
物理化学
分子
催化作用
有机化学
作者
Bo Wen,Mauro Andrade,Limin Liu,Annabella Selloni
标识
DOI:10.1073/pnas.2212250120
摘要
The interaction of water with TiO 2 surfaces is of crucial importance in various scientific fields and applications, from photocatalysis for hydrogen production and the photooxidation of organic pollutants to self-cleaning surfaces and bio-medical devices. In particular, the equilibrium fraction of water dissociation at the TiO 2 –water interface has a critical role in the surface chemistry of TiO 2 , but is difficult to determine both experimentally and computationally. Among TiO 2 surfaces, rutile TiO 2 (110) is of special interest as the most abundant surface of TiO 2 ’s stable rutile phase. While surface-science studies have provided detailed information on the interaction of rutile TiO 2 (110) with gas-phase water, much less is known about the TiO 2 (110)–water interface, which is more relevant to many applications. In this work, we characterize the structure of the aqueous TiO 2 (110) interface using nanosecond timescale molecular dynamics simulations with ab initio-based deep neural network potentials that accurately describe water/TiO 2 (110) interactions over a wide range of water coverages. Simulations on TiO 2 (110) slab models of increasing thickness provide insight into the dynamic equilibrium between molecular and dissociated adsorbed water at the interface and allow us to obtain a reliable estimate of the equilibrium fraction of water dissociation. We find a dissociation fraction of 22 ± 6% with an associated average hydroxyl lifetime of 7.6 ± 1.8 ns . These quantities are both much larger than corresponding estimates for the aqueous anatase TiO 2 (101) interface, consistent with the higher water photooxidation activity that is observed for rutile relative to anatase.
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