4.8 Article

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

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NATURE COMMUNICATIONS
卷 11, 期 1, 页码 -

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NATURE PORTFOLIO
DOI: 10.1038/s41467-020-15445-z

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资金

  1. Australian Research Council (ARC) [FL140100081]
  2. UK Catalysis Hub Consortium
  3. EPSRC [EP/R026939/1, EP/R026815/1, EP/R026645/1, EP/R027129/1, EP/M013219/1]
  4. Australian Synchrotron
  5. International Synchrotron Access Program (ISAP)
  6. Australian Government
  7. GCRF START project [ST/R002754/1]
  8. Supercomputing Wales project - European Regional Development Fund (ERDF) via Welsh Government
  9. STFC Scientific Computing Department's SCARF cluster
  10. EPSRC [EP/R026815/1, EP/K005030/1, EP/R026645/1, EP/R026939/1, EP/N010531/1] Funding Source: UKRI
  11. STFC [ST/R002754/1] Funding Source: UKRI

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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.

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