Cu oxide clusters in zeolites and metal organic frameworks are able to oxidize stabilize clusters of few atoms that exhibit high reactivity towards activation of methane and its subsequent transformation to methanol. The present results show conclusively that trimeric Cu oxo clusters in rather constrained local environments are active and selective for partial oxidation of methane. Zeolites with mordenite and ZSM5 structure stabilize such clusters in 8-MR side pockets of H-MOR as well as the 10-membered ring channels of MFI in the form of [Cu3(µ-O)3]2+ clusters. Theory indicates that the radical character of the oxygen in the cluster is indispensable for sufficient activity. Alkali cations near such clusters drastically reduce the ability to activate methane by changing the electron distribution in the cluster. The reactivity of Co and Fe oxide clusters as well as the reactivity of multinuclear Cu coordination complexes and oxide clusters in metalorganic frameworks will be discussed as potential alternatives to [Cu3(µ-O)3]2+ clusters in zeolites.

Strategies to selectively oxidize methane to methanol

253rd National Meeting (2017)

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