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Direct O2 Activation on Gold/Metal Oxide Catalysts through a Unique Double Linear O[BOND]Au[BOND]O Structure

Authors

  • Dr. Keju Sun,

    Corresponding author
    1. Research Institute for Ubiquitous Energy Devices, National Institute of Advanced Industrial Science and Technology, 1-8-31, Midorigaoka, Ikeda, Osaka 563-8577 (Japan), Fax: (+81) 72-751-9714
    2. The Institute of Scientific and Industrial Research, Osaka University, 8-1 Mihogaoka, Ibaraki, Osaka 567-0047 (Japan)
    • Research Institute for Ubiquitous Energy Devices, National Institute of Advanced Industrial Science and Technology, 1-8-31, Midorigaoka, Ikeda, Osaka 563-8577 (Japan), Fax: (+81) 72-751-9714
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  • Dr. Masanori Kohyama,

    1. Research Institute for Ubiquitous Energy Devices, National Institute of Advanced Industrial Science and Technology, 1-8-31, Midorigaoka, Ikeda, Osaka 563-8577 (Japan), Fax: (+81) 72-751-9714
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  • Dr. Shingo Tanaka,

    1. Research Institute for Ubiquitous Energy Devices, National Institute of Advanced Industrial Science and Technology, 1-8-31, Midorigaoka, Ikeda, Osaka 563-8577 (Japan), Fax: (+81) 72-751-9714
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  • Prof. Dr. Seiji Takeda

    1. The Institute of Scientific and Industrial Research, Osaka University, 8-1 Mihogaoka, Ibaraki, Osaka 567-0047 (Japan)
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Abstract

Nanogold particles supported on metal oxide surfaces present unusually high catalytic performances in low-temperature oxidation reactions. Despite numerous studies on that matter, the molecular mechanism concerning O2 activation remains controversial. Aimed to identify the active sites for direct O2 activation on gold, a Au[BOND]O[BOND]O[BOND]Au structure was analyzed by Hückel theory. It was found that an increase of Au–O orbital interaction can significantly promote O2 adsorption and dissociation. Therefore, we constructed a realistic model with a unique double linear Os[BOND]Au[BOND]Oa structure at the perimeter of the Au/metal oxide interfaces, which was examined subsequently by DFT calculations. The double linear Os[BOND]Au[BOND]Oa structure exhibited high reactivity, with O2 dissociation barriers as low as 0.12 eV and 0.17 eV for Au/TiO2 and Au/CeO2 systems, respectively. The present work gives new insight into the reaction mechanism of low-temperature oxidation reactions on gold catalysts.

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