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Single-site trinuclear copper oxygen clusters in mordenite for selective conversion of methane to methanol

Copper-exchanged zeolites with mordenite structure mimic the nuclearity and reactivity of active sites in particulate methane monooxygenase, which are enzymes able to selectively oxidize methane to methanol. Here we show that the mordenite micropores provide a perfect confined environment for the hi...

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Autores principales: Grundner, Sebastian, Markovits, Monica A.C., Li, Guanna, Tromp, Moniek, Pidko, Evgeny A., Hensen, Emiel J.M., Jentys, Andreas, Sanchez-Sanchez, Maricruz, Lercher, Johannes A.
Formato: Online Artículo Texto
Lenguaje:English
Publicado: Nature Pub. Group 2015
Materias:
Acceso en línea:https://www.ncbi.nlm.nih.gov/pmc/articles/PMC4491810/
https://www.ncbi.nlm.nih.gov/pubmed/26109507
http://dx.doi.org/10.1038/ncomms8546
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author Grundner, Sebastian
Markovits, Monica A.C.
Li, Guanna
Tromp, Moniek
Pidko, Evgeny A.
Hensen, Emiel J.M.
Jentys, Andreas
Sanchez-Sanchez, Maricruz
Lercher, Johannes A.
author_facet Grundner, Sebastian
Markovits, Monica A.C.
Li, Guanna
Tromp, Moniek
Pidko, Evgeny A.
Hensen, Emiel J.M.
Jentys, Andreas
Sanchez-Sanchez, Maricruz
Lercher, Johannes A.
author_sort Grundner, Sebastian
collection PubMed
description Copper-exchanged zeolites with mordenite structure mimic the nuclearity and reactivity of active sites in particulate methane monooxygenase, which are enzymes able to selectively oxidize methane to methanol. Here we show that the mordenite micropores provide a perfect confined environment for the highly selective stabilization of trinuclear copper-oxo clusters that exhibit a high reactivity towards activation of carbon–hydrogen bonds in methane and its subsequent transformation to methanol. The similarity with the enzymatic systems is also implied from the similarity of the reversible rearrangements of the trinuclear clusters occurring during the selective transformations of methane along the reaction path towards methanol, in both the enzyme system and copper-exchanged mordenite.
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spelling pubmed-44918102015-07-08 Single-site trinuclear copper oxygen clusters in mordenite for selective conversion of methane to methanol Grundner, Sebastian Markovits, Monica A.C. Li, Guanna Tromp, Moniek Pidko, Evgeny A. Hensen, Emiel J.M. Jentys, Andreas Sanchez-Sanchez, Maricruz Lercher, Johannes A. Nat Commun Article Copper-exchanged zeolites with mordenite structure mimic the nuclearity and reactivity of active sites in particulate methane monooxygenase, which are enzymes able to selectively oxidize methane to methanol. Here we show that the mordenite micropores provide a perfect confined environment for the highly selective stabilization of trinuclear copper-oxo clusters that exhibit a high reactivity towards activation of carbon–hydrogen bonds in methane and its subsequent transformation to methanol. The similarity with the enzymatic systems is also implied from the similarity of the reversible rearrangements of the trinuclear clusters occurring during the selective transformations of methane along the reaction path towards methanol, in both the enzyme system and copper-exchanged mordenite. Nature Pub. Group 2015-06-25 /pmc/articles/PMC4491810/ /pubmed/26109507 http://dx.doi.org/10.1038/ncomms8546 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
Grundner, Sebastian
Markovits, Monica A.C.
Li, Guanna
Tromp, Moniek
Pidko, Evgeny A.
Hensen, Emiel J.M.
Jentys, Andreas
Sanchez-Sanchez, Maricruz
Lercher, Johannes A.
Single-site trinuclear copper oxygen clusters in mordenite for selective conversion of methane to methanol
title Single-site trinuclear copper oxygen clusters in mordenite for selective conversion of methane to methanol
title_full Single-site trinuclear copper oxygen clusters in mordenite for selective conversion of methane to methanol
title_fullStr Single-site trinuclear copper oxygen clusters in mordenite for selective conversion of methane to methanol
title_full_unstemmed Single-site trinuclear copper oxygen clusters in mordenite for selective conversion of methane to methanol
title_short Single-site trinuclear copper oxygen clusters in mordenite for selective conversion of methane to methanol
title_sort single-site trinuclear copper oxygen clusters in mordenite for selective conversion of methane to methanol
topic Article
url https://www.ncbi.nlm.nih.gov/pmc/articles/PMC4491810/
https://www.ncbi.nlm.nih.gov/pubmed/26109507
http://dx.doi.org/10.1038/ncomms8546
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