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Synergistic ultraviolet and visible light photo-activation enables intensified low-temperature methanol synthesis over copper/zinc oxide/alumina

Author

Listed:
  • Bingqiao Xie

    (UNSW Australia)

  • Roong Jien Wong

    (RMIT University
    UK Catalysis Hub, Research Complex at Harwell, Rutherford Appleton Laboratory, Harwell)

  • Tze Hao Tan

    (UNSW Australia)

  • Michael Higham

    (UK Catalysis Hub, Research Complex at Harwell, Rutherford Appleton Laboratory, Harwell
    Cardiff University, Park Place)

  • Emma K. Gibson

    (UK Catalysis Hub, Research Complex at Harwell, Rutherford Appleton Laboratory, Harwell
    University of Glasgow)

  • Donato Decarolis

    (UK Catalysis Hub, Research Complex at Harwell, Rutherford Appleton Laboratory, Harwell
    Cardiff University, Park Place)

  • June Callison

    (UK Catalysis Hub, Research Complex at Harwell, Rutherford Appleton Laboratory, Harwell
    Cardiff University, Park Place)

  • Kondo-Francois Aguey-Zinsou

    (UNSW Australia)

  • Michael Bowker

    (UK Catalysis Hub, Research Complex at Harwell, Rutherford Appleton Laboratory, Harwell
    Cardiff University, Park Place)

  • C. Richard A. Catlow

    (UK Catalysis Hub, Research Complex at Harwell, Rutherford Appleton Laboratory, Harwell
    Cardiff University, Park Place
    University College London)

  • Jason Scott

    (UNSW Australia)

  • Rose Amal

    (UNSW Australia)

Abstract

Although photoexcitation has been employed to unlock the low-temperature equilibrium regimes of thermal catalysis, mechanism underlining potential interplay between electron excitations and surface chemical processes remains elusive. Here, we report an associative zinc oxide band-gap excitation and copper plasmonic excitation that can cooperatively promote methanol-production at the copper-zinc oxide interfacial perimeter of copper/zinc oxide/alumina (CZA) catalyst. Conversely, selective excitation of individual components only leads to the promotion of carbon monoxide production. Accompanied by the variation in surface copper oxidation state and local electronic structure of zinc, electrons originating from the zinc oxide excitation and copper plasmonic excitation serve to activate surface adsorbates, catalysing key elementary processes (namely formate conversion and hydrogen molecule activation), thus providing one explanation for the observed photothermal activity. These observations give valuable insights into the key elementary processes occurring on the surface of the CZA catalyst under light-heat dual activation.

Suggested Citation

  • Bingqiao Xie & Roong Jien Wong & Tze Hao Tan & Michael Higham & Emma K. Gibson & Donato Decarolis & June Callison & Kondo-Francois Aguey-Zinsou & Michael Bowker & C. Richard A. Catlow & Jason Scott & , 2020. "Synergistic ultraviolet and visible light photo-activation enables intensified low-temperature methanol synthesis over copper/zinc oxide/alumina," Nature Communications, Nature, vol. 11(1), pages 1-11, December.
  • Handle: RePEc:nat:natcom:v:11:y:2020:i:1:d:10.1038_s41467-020-15445-z
    DOI: 10.1038/s41467-020-15445-z
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    Cited by:

    1. Lu, Buchu & Yan, Xiangyu & Liu, Qibin, 2023. "Enhanced solar hydrogen generation with the direct coupling of photo and thermal energy – An experimental and mechanism study," Applied Energy, Elsevier, vol. 331(C).
    2. Zeshu Zhang & Chengliang Mao & Débora Motta Meira & Paul N. Duchesne & Athanasios A. Tountas & Zhao Li & Chenyue Qiu & Sanli Tang & Rui Song & Xue Ding & Junchuan Sun & Jiangfan Yu & Jane Y. Howe & We, 2022. "New black indium oxide—tandem photothermal CO2-H2 methanol selective catalyst," Nature Communications, Nature, vol. 13(1), pages 1-8, December.
    3. Yaguang Li & Xianhua Bai & Dachao Yuan & Fengyu Zhang & Bo Li & Xingyuan San & Baolai Liang & Shufang Wang & Jun Luo & Guangsheng Fu, 2022. "General heterostructure strategy of photothermal materials for scalable solar-heating hydrogen production without the consumption of artificial energy," Nature Communications, Nature, vol. 13(1), pages 1-10, December.

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