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Mesoporous MnCeO(x) solid solutions for low temperature and selective oxidation of hydrocarbons

The development of noble-metal-free heterogeneous catalysts that can realize the aerobic oxidation of C–H bonds at low temperature is a profound challenge in the catalysis community. Here we report the synthesis of a mesoporous Mn(0.5)Ce(0.5)O(x) solid solution that is highly active for the selectiv...

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Autores principales: Zhang, Pengfei, Lu, Hanfeng, Zhou, Ying, Zhang, Li, Wu, Zili, Yang, Shize, Shi, Hongliang, Zhu, Qiulian, Chen, Yinfei, Dai, Sheng
Formato: Online Artículo Texto
Lenguaje:English
Publicado: Nature Pub. Group 2015
Materias:
Acceso en línea:https://www.ncbi.nlm.nih.gov/pmc/articles/PMC4633985/
https://www.ncbi.nlm.nih.gov/pubmed/26469151
http://dx.doi.org/10.1038/ncomms9446
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author Zhang, Pengfei
Lu, Hanfeng
Zhou, Ying
Zhang, Li
Wu, Zili
Yang, Shize
Shi, Hongliang
Zhu, Qiulian
Chen, Yinfei
Dai, Sheng
author_facet Zhang, Pengfei
Lu, Hanfeng
Zhou, Ying
Zhang, Li
Wu, Zili
Yang, Shize
Shi, Hongliang
Zhu, Qiulian
Chen, Yinfei
Dai, Sheng
author_sort Zhang, Pengfei
collection PubMed
description The development of noble-metal-free heterogeneous catalysts that can realize the aerobic oxidation of C–H bonds at low temperature is a profound challenge in the catalysis community. Here we report the synthesis of a mesoporous Mn(0.5)Ce(0.5)O(x) solid solution that is highly active for the selective oxidation of hydrocarbons under mild conditions (100–120 °C). Notably, the catalytic performance achieved in the oxidation of cyclohexane to cyclohexanone/cyclohexanol (100 °C, conversion: 17.7%) is superior to those by the state-of-art commercial catalysts (140–160 °C, conversion: 3-5%). The high activity can be attributed to the formation of a Mn(0.5)Ce(0.5)O(x) solid solution with an ultrahigh manganese doping concentration in the CeO(2) cubic fluorite lattice, leading to maximum active surface oxygens for the activation of C–H bonds and highly reducible Mn(4+) ions for the rapid migration of oxygen vacancies from the bulk to the surface.
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spelling pubmed-46339852015-11-25 Mesoporous MnCeO(x) solid solutions for low temperature and selective oxidation of hydrocarbons Zhang, Pengfei Lu, Hanfeng Zhou, Ying Zhang, Li Wu, Zili Yang, Shize Shi, Hongliang Zhu, Qiulian Chen, Yinfei Dai, Sheng Nat Commun Article The development of noble-metal-free heterogeneous catalysts that can realize the aerobic oxidation of C–H bonds at low temperature is a profound challenge in the catalysis community. Here we report the synthesis of a mesoporous Mn(0.5)Ce(0.5)O(x) solid solution that is highly active for the selective oxidation of hydrocarbons under mild conditions (100–120 °C). Notably, the catalytic performance achieved in the oxidation of cyclohexane to cyclohexanone/cyclohexanol (100 °C, conversion: 17.7%) is superior to those by the state-of-art commercial catalysts (140–160 °C, conversion: 3-5%). The high activity can be attributed to the formation of a Mn(0.5)Ce(0.5)O(x) solid solution with an ultrahigh manganese doping concentration in the CeO(2) cubic fluorite lattice, leading to maximum active surface oxygens for the activation of C–H bonds and highly reducible Mn(4+) ions for the rapid migration of oxygen vacancies from the bulk to the surface. Nature Pub. Group 2015-10-15 /pmc/articles/PMC4633985/ /pubmed/26469151 http://dx.doi.org/10.1038/ncomms9446 Text en Copyright © 2015, Nature Publishing Group, a division of Macmillan Publishers Limited. All Rights Reserved. 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
Zhang, Pengfei
Lu, Hanfeng
Zhou, Ying
Zhang, Li
Wu, Zili
Yang, Shize
Shi, Hongliang
Zhu, Qiulian
Chen, Yinfei
Dai, Sheng
Mesoporous MnCeO(x) solid solutions for low temperature and selective oxidation of hydrocarbons
title Mesoporous MnCeO(x) solid solutions for low temperature and selective oxidation of hydrocarbons
title_full Mesoporous MnCeO(x) solid solutions for low temperature and selective oxidation of hydrocarbons
title_fullStr Mesoporous MnCeO(x) solid solutions for low temperature and selective oxidation of hydrocarbons
title_full_unstemmed Mesoporous MnCeO(x) solid solutions for low temperature and selective oxidation of hydrocarbons
title_short Mesoporous MnCeO(x) solid solutions for low temperature and selective oxidation of hydrocarbons
title_sort mesoporous mnceo(x) solid solutions for low temperature and selective oxidation of hydrocarbons
topic Article
url https://www.ncbi.nlm.nih.gov/pmc/articles/PMC4633985/
https://www.ncbi.nlm.nih.gov/pubmed/26469151
http://dx.doi.org/10.1038/ncomms9446
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