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Stable and solubilized active Au atom clusters for selective epoxidation of cis-cyclooctene with molecular oxygen
The ability of Au catalysts to effect the challenging task of utilizing molecular oxygen for the selective epoxidation of cyclooctene is fascinating. Although supported nanometre-size Au particles are poorly active, here we show that solubilized atomic Au clusters, present in ng ml(−1) concentration...
Autores principales: | , , , , , , , , |
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Formato: | Online Artículo Texto |
Lenguaje: | English |
Publicado: |
Nature Publishing Group
2017
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Materias: | |
Acceso en línea: | https://www.ncbi.nlm.nih.gov/pmc/articles/PMC5379066/ https://www.ncbi.nlm.nih.gov/pubmed/28348389 http://dx.doi.org/10.1038/ncomms14881 |
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author | Qian, Linping Wang, Zhen Beletskiy, Evgeny V. Liu, Jingyue dos Santos, Haroldo J. Li, Tiehu Rangel, Maria do C. Kung, Mayfair C. Kung, Harold H. |
author_facet | Qian, Linping Wang, Zhen Beletskiy, Evgeny V. Liu, Jingyue dos Santos, Haroldo J. Li, Tiehu Rangel, Maria do C. Kung, Mayfair C. Kung, Harold H. |
author_sort | Qian, Linping |
collection | PubMed |
description | The ability of Au catalysts to effect the challenging task of utilizing molecular oxygen for the selective epoxidation of cyclooctene is fascinating. Although supported nanometre-size Au particles are poorly active, here we show that solubilized atomic Au clusters, present in ng ml(−1) concentrations and stabilized by ligands derived from the oxidized hydrocarbon products, are active. They can be formed from various Au sources. They generate initiators and propagators to trigger the onset of the auto-oxidation reaction with an apparent turnover frequency of 440 s(−1), and continue to generate additional initiators throughout the auto-oxidation cycle without direct participation in the cycle. Spectroscopic characterization suggests that 7–8 atom clusters are effective catalytically. Extension of work based on these understandings leads to the demonstration that these Au clusters are also effective in selective oxidation of cyclohexene, and that solubilized Pt clusters are also capable of generating initiators for cyclooctene epoxidation. |
format | Online Article Text |
id | pubmed-5379066 |
institution | National Center for Biotechnology Information |
language | English |
publishDate | 2017 |
publisher | Nature Publishing Group |
record_format | MEDLINE/PubMed |
spelling | pubmed-53790662017-04-11 Stable and solubilized active Au atom clusters for selective epoxidation of cis-cyclooctene with molecular oxygen Qian, Linping Wang, Zhen Beletskiy, Evgeny V. Liu, Jingyue dos Santos, Haroldo J. Li, Tiehu Rangel, Maria do C. Kung, Mayfair C. Kung, Harold H. Nat Commun Article The ability of Au catalysts to effect the challenging task of utilizing molecular oxygen for the selective epoxidation of cyclooctene is fascinating. Although supported nanometre-size Au particles are poorly active, here we show that solubilized atomic Au clusters, present in ng ml(−1) concentrations and stabilized by ligands derived from the oxidized hydrocarbon products, are active. They can be formed from various Au sources. They generate initiators and propagators to trigger the onset of the auto-oxidation reaction with an apparent turnover frequency of 440 s(−1), and continue to generate additional initiators throughout the auto-oxidation cycle without direct participation in the cycle. Spectroscopic characterization suggests that 7–8 atom clusters are effective catalytically. Extension of work based on these understandings leads to the demonstration that these Au clusters are also effective in selective oxidation of cyclohexene, and that solubilized Pt clusters are also capable of generating initiators for cyclooctene epoxidation. Nature Publishing Group 2017-03-28 /pmc/articles/PMC5379066/ /pubmed/28348389 http://dx.doi.org/10.1038/ncomms14881 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 Qian, Linping Wang, Zhen Beletskiy, Evgeny V. Liu, Jingyue dos Santos, Haroldo J. Li, Tiehu Rangel, Maria do C. Kung, Mayfair C. Kung, Harold H. Stable and solubilized active Au atom clusters for selective epoxidation of cis-cyclooctene with molecular oxygen |
title | Stable and solubilized active Au atom clusters for selective epoxidation of cis-cyclooctene with molecular oxygen |
title_full | Stable and solubilized active Au atom clusters for selective epoxidation of cis-cyclooctene with molecular oxygen |
title_fullStr | Stable and solubilized active Au atom clusters for selective epoxidation of cis-cyclooctene with molecular oxygen |
title_full_unstemmed | Stable and solubilized active Au atom clusters for selective epoxidation of cis-cyclooctene with molecular oxygen |
title_short | Stable and solubilized active Au atom clusters for selective epoxidation of cis-cyclooctene with molecular oxygen |
title_sort | stable and solubilized active au atom clusters for selective epoxidation of cis-cyclooctene with molecular oxygen |
topic | Article |
url | https://www.ncbi.nlm.nih.gov/pmc/articles/PMC5379066/ https://www.ncbi.nlm.nih.gov/pubmed/28348389 http://dx.doi.org/10.1038/ncomms14881 |
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