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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...
Autores principales: | , , , , , , , , , |
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Formato: | Online Artículo Texto |
Lenguaje: | English |
Publicado: |
Nature Pub. Group
2015
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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. |
format | Online Article Text |
id | pubmed-4633985 |
institution | National Center for Biotechnology Information |
language | English |
publishDate | 2015 |
publisher | Nature Pub. Group |
record_format | MEDLINE/PubMed |
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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