First-Principle Calculations of Solvated Electrons at Protic Solvent−TiO2 Interfaces with Oxygen Vacancies

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• 作者：Takanori Koitaya ; Hisao Nakamura ; Koichi Yamashita
• 刊名：Journal of Physical Chemistry C
• 出版年：2009
• 出版时间：April 30, 2009
• 年：2009
• 卷：113
• 期：17
• 页码：7236-7245
• 全文大小：321K
• 年卷期：v.113,no.17(April 30, 2009)
• ISSN：1932-7455

文摘

Heterogeneous electron transfer dynamics at molecule−metal or molecule−metal oxide interfaces are a central issue for many fields in surface science. Recent time-resolved two-photon photoemission studies observed electron solvation at protic molecule−metal or −metal oxide interfaces in photoinduced charge transfer processes. Although the solvated electron is expected as a functional state (for instance, highly catalytic active site, promoter of charge transfer at devices), details are not yet well understood because of the strong dependence of specific atomistic-level solvent−substrate interactions on interfaces, e.g., ordered hydrogen bonds or defects at surfaces. We focus on the interfaces of H₂O/TiO₂(110) and CH₃OH/TiO₂(110) and have applied ab initio DFT calculations for several structures with changing coverage and adsorption types and after inserting oxygen vacancies. The electronic structures of wet-electron states and hydrogen bonds at interfaces have been analyzed using the calculated results.