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

Journal Article · · Nature Communications
DOI:https://doi.org/10.1038/ncomms8546· OSTI ID:1454255
 [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)

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.

Research Organization:
Univ. of Minnesota, Minneapolis, MN (United States)
Sponsoring Organization:
USDOE Office of Science (SC), Basic Energy Sciences (BES)
Grant/Contract Number:
SC0012702
OSTI ID:
1454255
Journal Information:
Nature Communications, Vol. 6, Issue 1; ISSN 2041-1723
Publisher:
Nature Publishing GroupCopyright Statement
Country of Publication:
United States
Language:
English
Citation Metrics:
Cited by: 540 works
Citation information provided by
Web of Science

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The Effect of the Active-Site Structure on the Activity of Copper Mordenite in the Aerobic and Anaerobic Conversion of Methane into Methanol journal June 2018
The Direct Catalytic Oxidation of Methane to Methanol-A Critical Assessment journal November 2017
From Solar Energy to Fuels: Recent Advances in Light-Driven C 1 Chemistry journal September 2019
Improved Efficiency for Partial Oxidation of Methane by Controlled Copper Deposition on Surface-Modified ZSM-5 journal December 2015
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Aqueous‐Phase Selective Oxidation of Methane with Oxygen over Iron Salts and Pd/C in the Presence of Hydrogen journal July 2019
Zeolite Surface Methoxy Groups as Key Intermediates in the Stepwise Conversion of Methane to Methanol journal September 2019
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