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The reactivity of closed-shell gas phase cluster anions AuTi 3 O 7  - and AuTi 3 O 8  - with methane under thermal collision conditions was studied by mass spectrometric experiments and quantum chemical calculations. Methane activation was observed with the formation of AuCH 3 in both cases, while the formation of formaldehyde was also identified in the reaction system of AuTi 3 O 8  - . The cooperative effect of the separated Au + and O 2- ions on the clusters induces the cleavage of the first C-H bond of methane. Further activation of the second C-H bond by a peroxide ion O 2  2- leads to the formation of formaldehyde. This study shows that closed-shell species on metal oxides can be reactive enough to facilitate thermal H-CH 3 bond cleavage and the subsequent conversion.

Methane activation by gold-doped titanium oxide cluster anions with closed-shell electronic structures