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Title: 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:
 [1];  [1];  [2];  [3];  [2];  [2];  [1];  [1];  [4]
  1. Technische Univ. Munchen, Garching (Germany)
  2. Eindhoven Univ. of Technology, Eindhoven (The Netherlands)
  3. Univ. of Amsterdam, Amsterdam (The Netherlands)
  4. 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) (SC-22)
OSTI Identifier:
1454255
Grant/Contract Number:  
SC0012702
Resource Type:
Journal Article: 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. 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, and Lercher, Johannes A. Thu . "Single-site trinuclear copper oxygen clusters in mordenite for selective conversion of methane to methanol". United States. doi: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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Cited by: 114 works
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