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

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...

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Autores principales: Xie, Bingqiao, Wong, Roong Jien, Tan, Tze Hao, Higham, Michael, Gibson, Emma K., Decarolis, Donato, Callison, June, Aguey-Zinsou, Kondo-Francois, Bowker, Michael, Catlow, C. Richard A., Scott, Jason, Amal, Rose
Formato: Online Artículo Texto
Lenguaje:English
Publicado: Nature Publishing Group UK 2020
Materias:
Acceso en línea:https://www.ncbi.nlm.nih.gov/pmc/articles/PMC7109065/
https://www.ncbi.nlm.nih.gov/pubmed/32235859
http://dx.doi.org/10.1038/s41467-020-15445-z
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author Xie, Bingqiao
Wong, Roong Jien
Tan, Tze Hao
Higham, Michael
Gibson, Emma K.
Decarolis, Donato
Callison, June
Aguey-Zinsou, Kondo-Francois
Bowker, Michael
Catlow, C. Richard A.
Scott, Jason
Amal, Rose
author_facet Xie, Bingqiao
Wong, Roong Jien
Tan, Tze Hao
Higham, Michael
Gibson, Emma K.
Decarolis, Donato
Callison, June
Aguey-Zinsou, Kondo-Francois
Bowker, Michael
Catlow, C. Richard A.
Scott, Jason
Amal, Rose
author_sort Xie, Bingqiao
collection PubMed
description 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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spelling pubmed-71090652020-04-03 Synergistic ultraviolet and visible light photo-activation enables intensified low-temperature methanol synthesis over copper/zinc oxide/alumina Xie, Bingqiao Wong, Roong Jien Tan, Tze Hao Higham, Michael Gibson, Emma K. Decarolis, Donato Callison, June Aguey-Zinsou, Kondo-Francois Bowker, Michael Catlow, C. Richard A. Scott, Jason Amal, Rose Nat Commun Article 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. Nature Publishing Group UK 2020-03-31 /pmc/articles/PMC7109065/ /pubmed/32235859 http://dx.doi.org/10.1038/s41467-020-15445-z Text en © Crown 2020 Open Access This article is licensed under a Creative Commons Attribution 4.0 International License, which permits use, sharing, adaptation, distribution and reproduction in any medium or format, as long as you give appropriate credit to the original author(s) and the source, provide a link to the Creative Commons license, and indicate if changes were made. The images or other third party material in this article are included in the article’s Creative Commons license, unless indicated otherwise in a credit line to the material. If material is not included in the article’s Creative Commons license and your intended use is not permitted by statutory regulation or exceeds the permitted use, you will need to obtain permission directly from the copyright holder. To view a copy of this license, visit http://creativecommons.org/licenses/by/4.0/.
spellingShingle Article
Xie, Bingqiao
Wong, Roong Jien
Tan, Tze Hao
Higham, Michael
Gibson, Emma K.
Decarolis, Donato
Callison, June
Aguey-Zinsou, Kondo-Francois
Bowker, Michael
Catlow, C. Richard A.
Scott, Jason
Amal, Rose
Synergistic ultraviolet and visible light photo-activation enables intensified low-temperature methanol synthesis over copper/zinc oxide/alumina
title Synergistic ultraviolet and visible light photo-activation enables intensified low-temperature methanol synthesis over copper/zinc oxide/alumina
title_full Synergistic ultraviolet and visible light photo-activation enables intensified low-temperature methanol synthesis over copper/zinc oxide/alumina
title_fullStr Synergistic ultraviolet and visible light photo-activation enables intensified low-temperature methanol synthesis over copper/zinc oxide/alumina
title_full_unstemmed Synergistic ultraviolet and visible light photo-activation enables intensified low-temperature methanol synthesis over copper/zinc oxide/alumina
title_short Synergistic ultraviolet and visible light photo-activation enables intensified low-temperature methanol synthesis over copper/zinc oxide/alumina
title_sort synergistic ultraviolet and visible light photo-activation enables intensified low-temperature methanol synthesis over copper/zinc oxide/alumina
topic Article
url https://www.ncbi.nlm.nih.gov/pmc/articles/PMC7109065/
https://www.ncbi.nlm.nih.gov/pubmed/32235859
http://dx.doi.org/10.1038/s41467-020-15445-z
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