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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. 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.

SUBMITTER: Grundner S 

PROVIDER: S-EPMC4491810 | biostudies-other | 2015

REPOSITORIES: biostudies-other

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

Grundner Sebastian S   Markovits Monica A C MA   Li Guanna G   Tromp Moniek M   Pidko Evgeny A EA   Hensen Emiel J M EJ   Jentys Andreas A   Sanchez-Sanchez Maricruz M   Lercher Johannes A JA  

Nature communications 20150625


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  ...[more]

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