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Noncontact catalysis: Initiation of selective ethylbenzene oxidation by Au cluster-facilitated cyclooctene epoxidation

Traditionally, a catalyst functions by direct interaction with reactants. In a new noncontact catalytic system (NCCS), an intermediate produced by one catalytic reaction serves as an intermediary to enable an independent reaction to proceed. An example is the selective oxidation of ethylbenzene, whi...

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Autores principales: Peng, Anyang, Kung, Mayfair C., Brydon, Robert R. O., Ross, Matthew O., Qian, Linping, Broadbelt, Linda J., Kung, Harold H.
Formato: Online Artículo Texto
Lenguaje:English
Publicado: American Association for the Advancement of Science 2020
Materias:
Acceso en línea:https://www.ncbi.nlm.nih.gov/pmc/articles/PMC6994218/
https://www.ncbi.nlm.nih.gov/pubmed/32064337
http://dx.doi.org/10.1126/sciadv.aax6637
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author Peng, Anyang
Kung, Mayfair C.
Brydon, Robert R. O.
Ross, Matthew O.
Qian, Linping
Broadbelt, Linda J.
Kung, Harold H.
author_facet Peng, Anyang
Kung, Mayfair C.
Brydon, Robert R. O.
Ross, Matthew O.
Qian, Linping
Broadbelt, Linda J.
Kung, Harold H.
author_sort Peng, Anyang
collection PubMed
description Traditionally, a catalyst functions by direct interaction with reactants. In a new noncontact catalytic system (NCCS), an intermediate produced by one catalytic reaction serves as an intermediary to enable an independent reaction to proceed. An example is the selective oxidation of ethylbenzene, which could not occur in the presence of either solubilized Au nanoclusters or cyclooctene, but proceeded readily when both were present simultaneously. The Au-initiated selective epoxidation of cyclooctene generated cyclooctenyl peroxy and oxy radicals that served as intermediaries to initiate the ethylbenzene oxidation. This combined system effectively extended the catalytic effect of Au. The reaction mechanism was supported by reaction kinetics and spin trap experiments. NCCS enables parallel reactions to proceed without the constraints of stoichiometric relationships, offering new degrees of freedom in industrial hydrocarbon co-oxidation processes.
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spelling pubmed-69942182020-02-14 Noncontact catalysis: Initiation of selective ethylbenzene oxidation by Au cluster-facilitated cyclooctene epoxidation Peng, Anyang Kung, Mayfair C. Brydon, Robert R. O. Ross, Matthew O. Qian, Linping Broadbelt, Linda J. Kung, Harold H. Sci Adv Research Articles Traditionally, a catalyst functions by direct interaction with reactants. In a new noncontact catalytic system (NCCS), an intermediate produced by one catalytic reaction serves as an intermediary to enable an independent reaction to proceed. An example is the selective oxidation of ethylbenzene, which could not occur in the presence of either solubilized Au nanoclusters or cyclooctene, but proceeded readily when both were present simultaneously. The Au-initiated selective epoxidation of cyclooctene generated cyclooctenyl peroxy and oxy radicals that served as intermediaries to initiate the ethylbenzene oxidation. This combined system effectively extended the catalytic effect of Au. The reaction mechanism was supported by reaction kinetics and spin trap experiments. NCCS enables parallel reactions to proceed without the constraints of stoichiometric relationships, offering new degrees of freedom in industrial hydrocarbon co-oxidation processes. American Association for the Advancement of Science 2020-01-31 /pmc/articles/PMC6994218/ /pubmed/32064337 http://dx.doi.org/10.1126/sciadv.aax6637 Text en Copyright © 2020 The Authors, some rights reserved; exclusive licensee American Association for the Advancement of Science. No claim to original U.S. Government Works. Distributed under a Creative Commons Attribution NonCommercial License 4.0 (CC BY-NC). http://creativecommons.org/licenses/by-nc/4.0/ This is an open-access article distributed under the terms of the Creative Commons Attribution-NonCommercial license (http://creativecommons.org/licenses/by-nc/4.0/) , which permits use, distribution, and reproduction in any medium, so long as the resultant use is not for commercial advantage and provided the original work is properly cited.
spellingShingle Research Articles
Peng, Anyang
Kung, Mayfair C.
Brydon, Robert R. O.
Ross, Matthew O.
Qian, Linping
Broadbelt, Linda J.
Kung, Harold H.
Noncontact catalysis: Initiation of selective ethylbenzene oxidation by Au cluster-facilitated cyclooctene epoxidation
title Noncontact catalysis: Initiation of selective ethylbenzene oxidation by Au cluster-facilitated cyclooctene epoxidation
title_full Noncontact catalysis: Initiation of selective ethylbenzene oxidation by Au cluster-facilitated cyclooctene epoxidation
title_fullStr Noncontact catalysis: Initiation of selective ethylbenzene oxidation by Au cluster-facilitated cyclooctene epoxidation
title_full_unstemmed Noncontact catalysis: Initiation of selective ethylbenzene oxidation by Au cluster-facilitated cyclooctene epoxidation
title_short Noncontact catalysis: Initiation of selective ethylbenzene oxidation by Au cluster-facilitated cyclooctene epoxidation
title_sort noncontact catalysis: initiation of selective ethylbenzene oxidation by au cluster-facilitated cyclooctene epoxidation
topic Research Articles
url https://www.ncbi.nlm.nih.gov/pmc/articles/PMC6994218/
https://www.ncbi.nlm.nih.gov/pubmed/32064337
http://dx.doi.org/10.1126/sciadv.aax6637
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