Regensburg 2019 – wissenschaftliches Programm
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MM: Fachverband Metall- und Materialphysik
MM 20: Poster session II
MM 20.27: Poster
Dienstag, 2. April 2019, 18:30–20:00, Poster C
Activation of methane and carbon dioxide by cationic tantalum clusters and their oxides under multi-collision conditions — •Theresa Zach, Nikita Levin, Jozef Lengyel, Martin Tschurl, and Ueli Heiz — Chair of Physical Chemistry, Department of Chemistry and Catalysis Research Center, Technical University of Munich, Lichtenbergstr. 4, 85748 Garching, Germany
The conversion of methane and carbon dioxide, potent greenhouse gases, to value-added products is considered as one the most desirable reactions in chemistry. Tantalum-based clusters exhibit promising properties on the activation of methane and carbon dioxide. The goal of our experiment is to investigate the complex reaction mechanisms using kinetic modeling in different size regimes, from the bare atom to clusters containing tens of atoms. Both reactions are measured experimentally in the gas-phase by ion trap mass spectrometry under multi-collisional conditions, which allow us to study the kinetics of the reactions as a function of temperature, which is essential to determine the corresponding activation energies. Using this setup for clusters of different sizes and oxidation states, we have surprisingly observed very promising catalytic activity of [Ta8O2]+ in reaction with CH4. The results suggest that the initial dehydrogenation of CH4 to form [Ta8O2CH2]+ is in consecutive reaction with additional CH4 yielding [Ta8O2C2H6]+. Ta8O2+ is then regenerated via release of the ethane. Further we intent to investigate the reactivity of Tan+ clusters towards CO2. The preliminary results of these experiments will be presented at the conference.