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

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 () and Rose Amal ()
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Bingqiao Xie: UNSW Australia
Roong Jien Wong: RMIT University
Tze Hao Tan: UNSW Australia
Michael Higham: UK Catalysis Hub, Research Complex at Harwell, Rutherford Appleton Laboratory, Harwell
Emma K. Gibson: UK Catalysis Hub, Research Complex at Harwell, Rutherford Appleton Laboratory, Harwell
Donato Decarolis: UK Catalysis Hub, Research Complex at Harwell, Rutherford Appleton Laboratory, Harwell
June Callison: UK Catalysis Hub, Research Complex at Harwell, Rutherford Appleton Laboratory, Harwell
Kondo-Francois Aguey-Zinsou: UNSW Australia
Michael Bowker: UK Catalysis Hub, Research Complex at Harwell, Rutherford Appleton Laboratory, Harwell
C. Richard A. Catlow: UK Catalysis Hub, Research Complex at Harwell, Rutherford Appleton Laboratory, Harwell
Jason Scott: UNSW Australia
Rose Amal: UNSW Australia

Nature Communications, 2020, vol. 11, issue 1, 1-11

Abstract: 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.

Date: 2020
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DOI: 10.1038/s41467-020-15445-z

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