Hydrogen-Bond Bridged Water Oxidation on {001} Surfaces of Anatase TiO2

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• 作者：Hongna Zhang ; Peng Zhou ; Zuofeng Chen ; Wenjing Song ; Hongwei Ji ; Wanhong Ma ; Chuncheng ChenJincai Zhao
• 刊名：Journal of Physical Chemistry C
• 出版年：2017
• 出版时间：February 2, 2017
• 年：2017
• 卷：121
• 期：4
• 页码：2251-2257
• 全文大小：406K
• ISSN：1932-7455

文摘

To gain an atomic-level understanding of the relationship among the surface structure, the interfacial interaction, and the water oxidation activity on TiO₂, we studied the adsorption of water and its photocatalytic oxidation on anatase TiO₂ with {101} and {001} exposed surfaces by in situ infrared spectroscopy, kinetic isotope effect studies, and density functional theory (DFT)-based molecular dynamics calculations. Our experimental results demonstrate that the oxidation reaction occurs exclusively on hydrogen-bonded water molecules (via surface hydroxyls) over {001} surface, whereas water molecules coordinated on the {101} surface, which are conventionally assigned to the reactive target for hole transfer, remain unchanged during the irradiation. The theoretical calculations reveal that the selective oxidation of water adsorbed on the {001} surfaces is primarily attributed to the formation of hydrogen bonds, which provides a channel to the rapid hole transfer and facilitates the O–H bond cleavage during water oxidation.