Single-site trinuclear copper oxygen clusters in mordenite for selective conversion of methane to methanol
Abstract
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. In conclusion, 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.
- Authors:
-
- Technische Univ. Munchen, Garching (Germany)
- Eindhoven Univ. of Technology, Eindhoven (The Netherlands)
- Univ. of Amsterdam, Amsterdam (The Netherlands)
- Technische Univ. Munchen, Garching (Germany); Pacific Northwest National Lab. (PNNL), Richland, WA (United States)
- Publication Date:
- Research Org.:
- Univ. of Minnesota, Minneapolis, MN (United States)
- Sponsoring Org.:
- USDOE Office of Science (SC), Basic Energy Sciences (BES)
- OSTI Identifier:
- 1454255
- Grant/Contract Number:
- SC0012702
- Resource Type:
- Accepted Manuscript
- Journal Name:
- Nature Communications
- Additional Journal Information:
- Journal Volume: 6; Journal Issue: 1; Journal ID: ISSN 2041-1723
- Publisher:
- Nature Publishing Group
- Country of Publication:
- United States
- Language:
- English
- Subject:
- 37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY
Citation Formats
Grundner, Sebastian, Markovits, Monica A. C., Li, Guanna, Tromp, Moniek, Pidko, Evgeny A., Hensen, Emiel J. M., Jentys, Andreas, Sanchez-Sanchez, Maricruz, and Lercher, Johannes A. Single-site trinuclear copper oxygen clusters in mordenite for selective conversion of methane to methanol. United States: N. p., 2015.
Web. doi:10.1038/ncomms8546.
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. United States. https://doi.org/10.1038/ncomms8546
Grundner, Sebastian, Markovits, Monica A. C., Li, Guanna, Tromp, Moniek, Pidko, Evgeny A., Hensen, Emiel J. M., Jentys, Andreas, Sanchez-Sanchez, Maricruz, and Lercher, Johannes A. Thu .
"Single-site trinuclear copper oxygen clusters in mordenite for selective conversion of methane to methanol". United States. https://doi.org/10.1038/ncomms8546. https://www.osti.gov/servlets/purl/1454255.
@article{osti_1454255,
title = {Single-site trinuclear copper oxygen clusters in mordenite for selective conversion of methane to methanol},
author = {Grundner, Sebastian and Markovits, Monica A. C. and Li, Guanna and Tromp, Moniek and Pidko, Evgeny A. and Hensen, Emiel J. M. and Jentys, Andreas and Sanchez-Sanchez, Maricruz and Lercher, Johannes A.},
abstractNote = {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. In conclusion, 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.},
doi = {10.1038/ncomms8546},
journal = {Nature Communications},
number = 1,
volume = 6,
place = {United States},
year = {Thu Jun 25 00:00:00 EDT 2015},
month = {Thu Jun 25 00:00:00 EDT 2015}
}
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