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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...
Autores principales: | , , , , , , , , , , , |
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Formato: | Online Artículo Texto |
Lenguaje: | English |
Publicado: |
Nature Publishing Group UK
2020
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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. |
format | Online Article Text |
id | pubmed-7109065 |
institution | National Center for Biotechnology Information |
language | English |
publishDate | 2020 |
publisher | Nature Publishing Group UK |
record_format | MEDLINE/PubMed |
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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