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Au–Pd separation enhances bimetallic catalysis of alcohol oxidation

Author

Listed:
  • Xiaoyang Huang

    (Cardiff Catalysis Institute, School of Chemistry, Cardiff University)

  • Ouardia Akdim

    (Cardiff Catalysis Institute, School of Chemistry, Cardiff University)

  • Mark Douthwaite

    (Cardiff Catalysis Institute, School of Chemistry, Cardiff University)

  • Kai Wang

    (Cardiff Catalysis Institute, School of Chemistry, Cardiff University)

  • Liang Zhao

    (Cardiff Catalysis Institute, School of Chemistry, Cardiff University)

  • Richard J. Lewis

    (Cardiff Catalysis Institute, School of Chemistry, Cardiff University)

  • Samuel Pattisson

    (Cardiff Catalysis Institute, School of Chemistry, Cardiff University)

  • Isaac T. Daniel

    (Cardiff Catalysis Institute, School of Chemistry, Cardiff University)

  • Peter J. Miedziak

    (Cardiff Catalysis Institute, School of Chemistry, Cardiff University
    University of South Wales)

  • Greg Shaw

    (Cardiff Catalysis Institute, School of Chemistry, Cardiff University)

  • David J. Morgan

    (Cardiff Catalysis Institute, School of Chemistry, Cardiff University)

  • Sultan M. Althahban

    (Lehigh University
    Jazan University)

  • Thomas E. Davies

    (Cardiff Catalysis Institute, School of Chemistry, Cardiff University)

  • Qian He

    (Cardiff Catalysis Institute, School of Chemistry, Cardiff University
    National University of Singapore)

  • Fei Wang

    (Cardiff Catalysis Institute, School of Chemistry, Cardiff University)

  • Jile Fu

    (Cardiff Catalysis Institute, School of Chemistry, Cardiff University)

  • Donald Bethell

    (Cardiff Catalysis Institute, School of Chemistry, Cardiff University)

  • Steven McIntosh

    (Lehigh University)

  • Christopher J. Kiely

    (Lehigh University
    Lehigh University)

  • Graham J. Hutchings

    (Cardiff Catalysis Institute, School of Chemistry, Cardiff University)

Abstract

In oxidation reactions catalysed by supported metal nanoparticles with oxygen as the terminal oxidant, the rate of the oxygen reduction can be a limiting factor. This is exemplified by the oxidative dehydrogenation of alcohols, an important class of reactions with modern commercial applications1–3. Supported gold nanoparticles are highly active for the dehydrogenation of the alcohol to an aldehyde4 but are less effective for oxygen reduction5,6. By contrast, supported palladium nanoparticles offer high efficacy for oxygen reduction5,6. This imbalance can be overcome by alloying gold with palladium, which gives enhanced activity to both reactions7,8,9; however, the electrochemical potential of the alloy is a compromise between that of the two metals, meaning that although the oxygen reduction can be improved in the alloy, the dehydrogenation activity is often limited. Here we show that by separating the gold and palladium components in bimetallic carbon-supported catalysts, we can almost double the reaction rate compared with that achieved with the corresponding alloy catalyst. We demonstrate this using physical mixtures of carbon-supported monometallic gold and palladium catalysts and a bimetallic catalyst comprising separated gold and palladium regions. Furthermore, we demonstrate electrochemically that this enhancement is attributable to the coupling of separate redox processes occurring at isolated gold and palladium sites. The discovery of this catalytic effect—a cooperative redox enhancement—offers an approach to the design of multicomponent heterogeneous catalysts.

Suggested Citation

  • Xiaoyang Huang & Ouardia Akdim & Mark Douthwaite & Kai Wang & Liang Zhao & Richard J. Lewis & Samuel Pattisson & Isaac T. Daniel & Peter J. Miedziak & Greg Shaw & David J. Morgan & Sultan M. Althahban, 2022. "Au–Pd separation enhances bimetallic catalysis of alcohol oxidation," Nature, Nature, vol. 603(7900), pages 271-275, March.
  • Handle: RePEc:nat:nature:v:603:y:2022:i:7900:d:10.1038_s41586-022-04397-7
    DOI: 10.1038/s41586-022-04397-7
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    Cited by:

    1. Hui Su & Jing-Tan Han & Botong Miao & Mahdi Salehi & Chao-Jun Li, 2024. "Photosynthesis of CH3OH via oxygen-atom-grafting from CO2 to CH4 enabled by AuPd/GaN," Nature Communications, Nature, vol. 15(1), pages 1-9, December.
    2. Chunsong Li & Haochen Zhang & Wenxuan Liu & Lin Sheng & Mu-Jeng Cheng & Bingjun Xu & Guangsheng Luo & Qi Lu, 2024. "Efficient conversion of propane in a microchannel reactor at ambient conditions," Nature Communications, Nature, vol. 15(1), pages 1-10, December.
    3. Hua Zhou & Yue Ren & Bingxin Yao & Zhenhua Li & Ming Xu & Lina Ma & Xianggui Kong & Lirong Zheng & Mingfei Shao & Haohong Duan, 2023. "Scalable electrosynthesis of commodity chemicals from biomass by suppressing non-Faradaic transformations," Nature Communications, Nature, vol. 14(1), pages 1-12, December.

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