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Importance of Methane Chemical Potential for Its Conversion to Methanol on Cu‐Exchanged Mordenite

Copper‐oxo clusters exchanged in zeolite mordenite are active in the stoichiometric conversion of methane to methanol at low temperatures. Here, we show an unprecedented methanol yield per Cu of 0.6, with a 90–95 % selectivity, on a MOR solely containing [Cu(3)(μ‐O)(3)](2+) active sites. DFT calcula...

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Autores principales: Zheng, Jian, Lee, Insu, Khramenkova, Elena, Wang, Meng, Peng, Bo, Gutiérrez, Oliver Y., Fulton, John L., Camaioni, Donald M., Khare, Rachit, Jentys, Andreas, Haller, Gary L., Pidko, Evgeny A., Sanchez‐Sanchez, Maricruz, Lercher, Johannes A.
Formato: Online Artículo Texto
Lenguaje:English
Publicado: John Wiley and Sons Inc. 2020
Materias:
Acceso en línea:https://www.ncbi.nlm.nih.gov/pmc/articles/PMC7317825/
https://www.ncbi.nlm.nih.gov/pubmed/32092206
http://dx.doi.org/10.1002/chem.202000772
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author Zheng, Jian
Lee, Insu
Khramenkova, Elena
Wang, Meng
Peng, Bo
Gutiérrez, Oliver Y.
Fulton, John L.
Camaioni, Donald M.
Khare, Rachit
Jentys, Andreas
Haller, Gary L.
Pidko, Evgeny A.
Sanchez‐Sanchez, Maricruz
Lercher, Johannes A.
author_facet Zheng, Jian
Lee, Insu
Khramenkova, Elena
Wang, Meng
Peng, Bo
Gutiérrez, Oliver Y.
Fulton, John L.
Camaioni, Donald M.
Khare, Rachit
Jentys, Andreas
Haller, Gary L.
Pidko, Evgeny A.
Sanchez‐Sanchez, Maricruz
Lercher, Johannes A.
author_sort Zheng, Jian
collection PubMed
description Copper‐oxo clusters exchanged in zeolite mordenite are active in the stoichiometric conversion of methane to methanol at low temperatures. Here, we show an unprecedented methanol yield per Cu of 0.6, with a 90–95 % selectivity, on a MOR solely containing [Cu(3)(μ‐O)(3)](2+) active sites. DFT calculations, spectroscopic characterization and kinetic analysis show that increasing the chemical potential of methane enables the utilization of two μ‐oxo bridge oxygen out of the three available in the tricopper‐oxo cluster structure. Methanol and methoxy groups are stabilized in parallel, leading to methanol desorption in the presence of water.
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spelling pubmed-73178252020-06-29 Importance of Methane Chemical Potential for Its Conversion to Methanol on Cu‐Exchanged Mordenite Zheng, Jian Lee, Insu Khramenkova, Elena Wang, Meng Peng, Bo Gutiérrez, Oliver Y. Fulton, John L. Camaioni, Donald M. Khare, Rachit Jentys, Andreas Haller, Gary L. Pidko, Evgeny A. Sanchez‐Sanchez, Maricruz Lercher, Johannes A. Chemistry Communications Copper‐oxo clusters exchanged in zeolite mordenite are active in the stoichiometric conversion of methane to methanol at low temperatures. Here, we show an unprecedented methanol yield per Cu of 0.6, with a 90–95 % selectivity, on a MOR solely containing [Cu(3)(μ‐O)(3)](2+) active sites. DFT calculations, spectroscopic characterization and kinetic analysis show that increasing the chemical potential of methane enables the utilization of two μ‐oxo bridge oxygen out of the three available in the tricopper‐oxo cluster structure. Methanol and methoxy groups are stabilized in parallel, leading to methanol desorption in the presence of water. John Wiley and Sons Inc. 2020-05-11 2020-06-18 /pmc/articles/PMC7317825/ /pubmed/32092206 http://dx.doi.org/10.1002/chem.202000772 Text en © 2020 The Authors. Published by Wiley-VCH Verlag GmbH & Co. KGaA. This is an open access article under the terms of the http://creativecommons.org/licenses/by-nc-nd/4.0/ License, which permits use and distribution in any medium, provided the original work is properly cited, the use is non‐commercial and no modifications or adaptations are made.
spellingShingle Communications
Zheng, Jian
Lee, Insu
Khramenkova, Elena
Wang, Meng
Peng, Bo
Gutiérrez, Oliver Y.
Fulton, John L.
Camaioni, Donald M.
Khare, Rachit
Jentys, Andreas
Haller, Gary L.
Pidko, Evgeny A.
Sanchez‐Sanchez, Maricruz
Lercher, Johannes A.
Importance of Methane Chemical Potential for Its Conversion to Methanol on Cu‐Exchanged Mordenite
title Importance of Methane Chemical Potential for Its Conversion to Methanol on Cu‐Exchanged Mordenite
title_full Importance of Methane Chemical Potential for Its Conversion to Methanol on Cu‐Exchanged Mordenite
title_fullStr Importance of Methane Chemical Potential for Its Conversion to Methanol on Cu‐Exchanged Mordenite
title_full_unstemmed Importance of Methane Chemical Potential for Its Conversion to Methanol on Cu‐Exchanged Mordenite
title_short Importance of Methane Chemical Potential for Its Conversion to Methanol on Cu‐Exchanged Mordenite
title_sort importance of methane chemical potential for its conversion to methanol on cu‐exchanged mordenite
topic Communications
url https://www.ncbi.nlm.nih.gov/pmc/articles/PMC7317825/
https://www.ncbi.nlm.nih.gov/pubmed/32092206
http://dx.doi.org/10.1002/chem.202000772
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