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Activation of Dodecanethiol-Capped Gold Catalysts for CO Oxidation by Treatment with KMnO4 or K2MnO4

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Abstract

Dodecanethiol-protected gold nanoparticles were deposited onto fumed SiO2 (Cab-O-Sil) via colloidal deposition. The catalyst was treated with a strongly oxidative KMnO4 or K2MnO4 solution. Low-temperature conversion in catalytic CO oxidation increased dramatically following the oxidative treatment and subsequent thermal activation at 300 °C to burn off residual organic species. On the other hand, the treatment with Fenton’s reagent did not lead to any positive effect. The influences of the average sizes of pre-synthesized gold particles (1.8, 2.1, 3.9, 9.9 nm) and the choice of different supports (SiO2, TiO2, C) were investigated, and relevant characterization using TG/DTG, XRD, TEM, EDX, and HAADF was conducted. The catalyst stability as a function of time on stream was also surveyed. This work establishes the beneficial effect of treating dodecanethiol-capped gold catalysts by KMnO4 or K2MnO4.

Graphical Abstract

Dodecanethiol-capped gold nanoparticles were deposited onto SiO2, TiO2, or carbon support, and the resulting catalysts were treated by aqueous KMnO4 or K2MnO4 followed by treatment in O2–He at 300 °C. The catalytic activity in low-temperature CO oxidation was increased due to the creation of Au–MnO x interfaces.

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Acknowledgements

Research sponsored by the Division of Chemical Sciences, Geosciences, and Biosciences, Office of Basic Energy Sciences, U.S. Department of Energy under contract DE-AC05-00OR22725 with Oak Ridge National Laboratory, managed and operated by UT-Battelle, LLC. This research was also supported by the appointment for H.F. Yin to the ORNL Research Associates Program, administered by Oak Ridge Associated Universities. The electron microscopy experiments were carried out at the Oak Ridge National Laboratory SHaRE User Facility, which is supported by the Division of Scientific User Facilities, DOE Office of Science, Basic Energy Sciences.

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Authors and Affiliations

  1. Chemical Sciences Division, Oak Ridge National Laboratory, Oak Ridge, TN, 37831, USA

    Hongfeng Yin & Sheng Dai

  2. Department of Environmental Science and Engineering, Fudan University, Shanghai, 200433, People’s Republic of China

    Zhen Ma

  3. Materials Science and Technology Division, Oak Ridge National Laboratory, Oak Ridge, TN, 37831, USA

    Miaofang Chi

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  1. Hongfeng Yin
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  2. Zhen Ma
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  3. Miaofang Chi
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  4. Sheng Dai
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Correspondence to Sheng Dai.

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Yin, H., Ma, Z., Chi, M. et al. Activation of Dodecanethiol-Capped Gold Catalysts for CO Oxidation by Treatment with KMnO4 or K2MnO4 . Catal Lett 136, 209–221 (2010). https://doi.org/10.1007/s10562-010-0316-1

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