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Catalytic Oxidation of Methanol to Formaldehyde by Mass-Selected Vanadium Oxide Clusters Supported on a TiO2(110) Surface

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Department of Chemistry and Biochemistry, University of California, Santa Barbara, California 93106-9510, United States
*E-mail: [email protected]. Tel.: +1-805-893-3393. Fax: +1-805-893-4120.
Cite this: J. Phys. Chem. A 2014, 118, 37, 8309–8313
Publication Date (Web):April 17, 2014
https://doi.org/10.1021/jp5011378
Copyright © 2014 American Chemical Society
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    Abstract

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    We report the results of a systematic study of the catalytic activity of mass-selected vanadium oxide clusters deposited on rutile TiO2 surfaces under ultrahigh vacuum (UHV) conditions. Our results show that supported V, VO, and VO2 clusters are not catalytically active for the oxidative dehydrogenation of methanol to formaldehyde but can be made catalytically active by postoxidation. In addition, we found that the postoxidized VO/TiO2 produces the most formaldehyde. Scanning tunneling microscopy (STM) imaging of the postoxidized VO/TiO2 reveals isolated clusters with height and width indicative of VO3 bound to the TiO2 surface. Our results are consistent with previous density functional theory (DFT) calculations that predict that VO3 will be produced by postoxidation of VO and that VO3/TiO2 is an active catalyst.

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    the ratio of the QMS signal at m/z = 29 to the signal at m/z = 31. This material is available free of charge via the Internet at http://pubs.acs.org.

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    14. Dongmin Yun, Yang Song, José E. Herrera. Supported Vanadium Oxide Clusters in Partial Oxidation Processes: Catalytic Consequences of Size and Electronic Structure. ChemCatChem 2017, 9 (19) , 3655-3669. https://doi.org/10.1002/cctc.201700503
    15. Fanglin Che, Su Ha, Jean‐Sabin McEwen. Catalytic Reaction Rates Controlled by Metal Oxidation State: C−H Bond Cleavage in Methane over Nickel‐Based Catalysts. Angewandte Chemie 2017, 129 (13) , 3611-3615. https://doi.org/10.1002/ange.201611796
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    17. Vasilii I. Avdeev, Alexander F. Bedilo. Molecular mechanism of propane oxidative dehydrogenation on surface oxygen radical sites of VO x /TiO2 catalysts. Research on Chemical Intermediates 2016, 42 (6) , 5237-5252. https://doi.org/10.1007/s11164-015-2355-0
    18. Yizhen Li, Jiaying Yu, Wei Li, Guoli Fan, Lan Yang, Feng Li. The promotional effect of surface defects on the catalytic performance of supported nickel-based catalysts. Physical Chemistry Chemical Physics 2016, 18 (9) , 6548-6558. https://doi.org/10.1039/C5CP07371E
    19. Anawat Thivasasith, Jakkapan Sirijaraensre, Pipat Khongpracha, Chompunuch Warakulwit, Bavornpon Jansang, Jumras Limtrakul. Reaction Mechanism of Methanol to Formaldehyde over Fe‐ and FeO‐Modified Graphene. ChemPhysChem 2015, 16 (5) , 986-992. https://doi.org/10.1002/cphc.201402702
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