Journal
JOURNAL OF THE AMERICAN CHEMICAL SOCIETY
Volume 134, Issue 32, Pages 13366-13373Publisher
AMER CHEMICAL SOC
DOI: 10.1021/ja304049x
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Funding
- Chinese Academy of Sciences
- National Science Foundation of China
- Chinese Ministry of Science and Technology
- National Natural Science Foundation of China [21173212]
- Chinese Academy of Sciences Visiting Professorships for Senior International Scientists
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We have investigated the photocatalysis of partially deuterated methanol (CD3OH) and H2O on TiO2(110) at 400 nm using a newly developed photocatalysis apparatus in combination with theoretical calculations. Photocatalyzed products, CD2O on Ti-sc sites, and H and D atoms on bridge-bonded oxygen (BBO) sites from CD3OH have been clearly detected, while no evidence of H2O photocatalysis was found. The experimental results show that dissociation of CD3OH on TiO2(110) occurs in a stepwise manner in which the O-H dissociation proceeds first and is then followed by C-D dissociation. Theoretical calculations indicate that the high reverse barrier to C-D recombination and the facile desorption of CD2O make photocatalytic methanol dissociation on TiO2(110) proceed efficiently. Theoretical results also reveal that the reverse reactions, i.e, O-H recombination after H2O photocatalytic dissociation on TiO2(110), may occur easily, thus inhibiting efficient photocatalytic water splitting.
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