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


Journal

Nature communications
ISSN: 2041-1723
Titre abrégé: Nat Commun
Pays: England
ID NLM: 101528555

Informations de publication

Date de publication:
31 Mar 2020
Historique:
received: 11 11 2019
accepted: 26 02 2020
entrez: 3 4 2020
pubmed: 3 4 2020
medline: 3 4 2020
Statut: epublish

Résumé

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.

Identifiants

pubmed: 32235859
doi: 10.1038/s41467-020-15445-z
pii: 10.1038/s41467-020-15445-z
pmc: PMC7109065
doi:

Types de publication

Journal Article

Langues

eng

Sous-ensembles de citation

IM

Pagination

1615

Subventions

Organisme : Department of Education and Training | Australian Research Council (ARC)
ID : FL140100081

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Auteurs

Bingqiao Xie (B)

School of Chemical Engineering, UNSW Australia, Sydney, NSW, 2052, Australia.

Roong Jien Wong (RJ)

Applied Chemistry and Environmental Science, School of Science, RMIT University, Melbourne, VIC, 3000, Australia.
UK Catalysis Hub, Research Complex at Harwell, Rutherford Appleton Laboratory, Harwell, Oxon, OX11 0FA, UK.

Tze Hao Tan (TH)

School of Chemical Engineering, UNSW Australia, Sydney, NSW, 2052, Australia.

Michael Higham (M)

UK Catalysis Hub, Research Complex at Harwell, Rutherford Appleton Laboratory, Harwell, Oxon, OX11 0FA, UK.
School of Chemistry, Cardiff University, Park Place, Cardiff, CF10 1AT, UK.

Emma K Gibson (EK)

UK Catalysis Hub, Research Complex at Harwell, Rutherford Appleton Laboratory, Harwell, Oxon, OX11 0FA, UK.
School of Chemistry, Joseph Black Building, University of Glasgow, Glasgow, G12 8QQ, UK.

Donato Decarolis (D)

UK Catalysis Hub, Research Complex at Harwell, Rutherford Appleton Laboratory, Harwell, Oxon, OX11 0FA, UK.
School of Chemistry, Cardiff University, Park Place, Cardiff, CF10 1AT, UK.

June Callison (J)

UK Catalysis Hub, Research Complex at Harwell, Rutherford Appleton Laboratory, Harwell, Oxon, OX11 0FA, UK.
School of Chemistry, Cardiff University, Park Place, Cardiff, CF10 1AT, UK.

Kondo-Francois Aguey-Zinsou (KF)

School of Chemical Engineering, UNSW Australia, Sydney, NSW, 2052, Australia.

Michael Bowker (M)

UK Catalysis Hub, Research Complex at Harwell, Rutherford Appleton Laboratory, Harwell, Oxon, OX11 0FA, UK.
School of Chemistry, Cardiff University, Park Place, Cardiff, CF10 1AT, UK.

C Richard A Catlow (CRA)

UK Catalysis Hub, Research Complex at Harwell, Rutherford Appleton Laboratory, Harwell, Oxon, OX11 0FA, UK.
School of Chemistry, Cardiff University, Park Place, Cardiff, CF10 1AT, UK.
Department of Chemistry, University College London, 20 Gordon St, London, WC1 HOAJ, UK.

Jason Scott (J)

School of Chemical Engineering, UNSW Australia, Sydney, NSW, 2052, Australia. jason.scott@unsw.edu.au.

Rose Amal (R)

School of Chemical Engineering, UNSW Australia, Sydney, NSW, 2052, Australia. r.amal@unsw.edu.au.

Classifications MeSH