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O: Fachverband Oberflächenphysik

O 7: Heterogeneous Catalysis: Experiment

O 7.4: Vortrag

Montag, 12. März 2018, 11:15–11:30, MA 141

Methane activation mediated by free tantalum cluster cations: reactivity governed by cluster size — •Tsugunosuke Masubuchi¹, Jan Eckhard¹, George Goddard^1,2, Martin Tschurl¹, Robert Barnett³, Uzi Landman³, and Ueli Heiz¹ — ¹Chair of Physical Chemistry, Department of Chemistry & Catalysis Research Center, Technische Universität München, Lichtenbergstr. 4, 85748 Garching, Germany — ²Department of Chemistry, Durham University, Durham, U.K. DH1 3LE — ³School of Physics Georgia Institute of Technology Atlanta, Georgia 30332-0430, U.S.A.

Methane activation, which involves C-H bond cleavage, is an important topic for versatile use of methane as a feedstock. Many efforts have been made to seek efficient C-H activation of methane in the non-scalable size regime. In this contribution, we report the reactivity of size-selected tantalum cluster cations toward methane molecules, which are investigated under multi-collision conditions. Under such conditions cluster ions are thermalized to desired temperatures, adjustable in a wide range, thus advantageous to explore reaction kinetics.

The mass spectrometric approach shows that tantalum clusters with a certain size exhibit hydrogen elimination from methane at room temperature. On the other hand, the number of the dehydrogenated molecules bound to the cluster changes with cluster size. This feature is associated with the formation of dehydrogenated products.