Abstract:
Activation of carbon dioxide and methane by tantalum-based charged metal clusters is studied in gas-phase kinetic and spectroscopic experiments. In these experiments, two regimes of the reactivity of tantalum clusters towards CO2, a catalytic cycle of non-oxidative coupling of CH4 by Ta8O2+, and C-C and C-O coupling reactions enabled by bare Ta+ and Ta4+ were identified. This work further corroborates the usefulness of gas-phase studies for catalysis.