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Metal/oxide interfacial effects on the selective oxidation of primary alcohols

A main obstacle in the rational development of heterogeneous catalysts is the difficulty in identifying active sites. Here we show metal/oxide interfacial sites are highly active for the oxidation of benzyl alcohol and other industrially important primary alcohols on a range of metals and oxides com...

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Autores principales: Zhao, Guofeng, Yang, Fan, Chen, Zongjia, Liu, Qingfei, Ji, Yongjun, Zhang, Yi, Niu, Zhiqiang, Mao, Junjie, Bao, Xinhe, Hu, Peijun, Li, Yadong
Formato: Online Artículo Texto
Lenguaje:English
Publicado: Nature Publishing Group 2017
Materias:
Acceso en línea:https://www.ncbi.nlm.nih.gov/pmc/articles/PMC5253635/
https://www.ncbi.nlm.nih.gov/pubmed/28098146
http://dx.doi.org/10.1038/ncomms14039
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author Zhao, Guofeng
Yang, Fan
Chen, Zongjia
Liu, Qingfei
Ji, Yongjun
Zhang, Yi
Niu, Zhiqiang
Mao, Junjie
Bao, Xinhe
Hu, Peijun
Li, Yadong
author_facet Zhao, Guofeng
Yang, Fan
Chen, Zongjia
Liu, Qingfei
Ji, Yongjun
Zhang, Yi
Niu, Zhiqiang
Mao, Junjie
Bao, Xinhe
Hu, Peijun
Li, Yadong
author_sort Zhao, Guofeng
collection PubMed
description A main obstacle in the rational development of heterogeneous catalysts is the difficulty in identifying active sites. Here we show metal/oxide interfacial sites are highly active for the oxidation of benzyl alcohol and other industrially important primary alcohols on a range of metals and oxides combinations. Scanning tunnelling microscopy together with density functional theory calculations on FeO/Pt(111) reveals that benzyl alcohol enriches preferentially at the oxygen-terminated FeO/Pt(111) interface and undergoes readily O–H and C–H dissociations with the aid of interfacial oxygen, which is also validated in the model study of Cu(2)O/Ag(111). We demonstrate that the interfacial effects are independent of metal or oxide sizes and the way by which the interfaces were constructed. It inspires us to inversely support nano-oxides on micro-metals to make the structure more stable against sintering while the number of active sites is not sacrificed. The catalyst lifetime, by taking the inverse design, is thereby significantly prolonged.
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spelling pubmed-52536352017-02-03 Metal/oxide interfacial effects on the selective oxidation of primary alcohols Zhao, Guofeng Yang, Fan Chen, Zongjia Liu, Qingfei Ji, Yongjun Zhang, Yi Niu, Zhiqiang Mao, Junjie Bao, Xinhe Hu, Peijun Li, Yadong Nat Commun Article A main obstacle in the rational development of heterogeneous catalysts is the difficulty in identifying active sites. Here we show metal/oxide interfacial sites are highly active for the oxidation of benzyl alcohol and other industrially important primary alcohols on a range of metals and oxides combinations. Scanning tunnelling microscopy together with density functional theory calculations on FeO/Pt(111) reveals that benzyl alcohol enriches preferentially at the oxygen-terminated FeO/Pt(111) interface and undergoes readily O–H and C–H dissociations with the aid of interfacial oxygen, which is also validated in the model study of Cu(2)O/Ag(111). We demonstrate that the interfacial effects are independent of metal or oxide sizes and the way by which the interfaces were constructed. It inspires us to inversely support nano-oxides on micro-metals to make the structure more stable against sintering while the number of active sites is not sacrificed. The catalyst lifetime, by taking the inverse design, is thereby significantly prolonged. Nature Publishing Group 2017-01-18 /pmc/articles/PMC5253635/ /pubmed/28098146 http://dx.doi.org/10.1038/ncomms14039 Text en Copyright © 2017, The Author(s) http://creativecommons.org/licenses/by/4.0/ This work is licensed under a Creative Commons Attribution 4.0 International License. The images or other third party material in this article are included in the article's Creative Commons license, unless indicated otherwise in the credit line; if the material is not included under the Creative Commons license, users will need to obtain permission from the license holder to reproduce the material. To view a copy of this license, visit http://creativecommons.org/licenses/by/4.0/
spellingShingle Article
Zhao, Guofeng
Yang, Fan
Chen, Zongjia
Liu, Qingfei
Ji, Yongjun
Zhang, Yi
Niu, Zhiqiang
Mao, Junjie
Bao, Xinhe
Hu, Peijun
Li, Yadong
Metal/oxide interfacial effects on the selective oxidation of primary alcohols
title Metal/oxide interfacial effects on the selective oxidation of primary alcohols
title_full Metal/oxide interfacial effects on the selective oxidation of primary alcohols
title_fullStr Metal/oxide interfacial effects on the selective oxidation of primary alcohols
title_full_unstemmed Metal/oxide interfacial effects on the selective oxidation of primary alcohols
title_short Metal/oxide interfacial effects on the selective oxidation of primary alcohols
title_sort metal/oxide interfacial effects on the selective oxidation of primary alcohols
topic Article
url https://www.ncbi.nlm.nih.gov/pmc/articles/PMC5253635/
https://www.ncbi.nlm.nih.gov/pubmed/28098146
http://dx.doi.org/10.1038/ncomms14039
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