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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Veröffentlicht in:Nature communications Jg. 6; H. 1; S. 7546
Hauptverfasser: 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.
Format: Journal Article
Sprache:Englisch
Veröffentlicht: London Nature Publishing Group UK 25.06.2015
Nature Publishing Group
Nature Pub. Group
Schlagworte:
119/118
639/638/263/406/77/603
639/638/440
Catalysis
Chemistry
Copper
Enzymes
Humanities and Social Sciences
INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY
Methane
Methanol
multidisciplinary
Oxidation
Science
Science (multidisciplinary)
Zeolites
Netherlands
ISSN:2041-1723, 2041-1723
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Zusammenfassung: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. Copper-exchanged zeolites with mordenite structure can mimic the active sites in particulate methane monooxygenase. Here, the authors show that mordenite micropores can stabilize trinuclear copper-oxo clusters that exhibit a high reactivity towards activation of carbon–hydrogen bonds in methane.
Bibliographie:ObjectType-Article-1
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SC0012702
USDOE Office of Science (SC), Basic Energy Sciences (BES)
ISSN:2041-1723
2041-1723
DOI:10.1038/ncomms8546