SAMOP 2021 – scientific programme
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MO: Fachverband Molekülphysik
MO 2: Cluster & Complexes
MO 2.3: Talk
Monday, September 20, 2021, 14:30–14:45, H2
N2 Cleavage by Tantalum Cluster under Cryo Conditions — •Daniela V. Fries, Matthias P. Klein, Annika Straßner, Maximilan Huber, Marc H. Prosenc, and Gereon Niedner-Schatteburg — TU Kaiserslautern, Kaiserslautern, Deutschland
As motivated by prior room temperature studies on Ta2+[1] we investigate larger Tan+ clusters (4<n<7) and their N2 adsorption and activation abilities by adsorption kinetics and infrared spectroscopy under cryo conditions compared with DFT calculations.
The model system Ta4+ appears to be of particular interest with regard to cryo N2 activation. Experimental results reveal peculiar details for the first and second adsorption kinetics, and the infrared signatures show no NN stretching bands in [Ta4(N2)1]+ and [Ta4(N2)2]+. This is consistent with cleavage of the first two adsorbed dinitrogen molecules and we unravel a multistep above edge across surface (AEAS) mechanism for the cleavage of first and second N2 adsorbates. Cleavage of the third N2 ligand is kinetically hindered. We recognize that substoichiometric N2 exposure allows for spontaneous activation by Ta4+, while higher N2 exposure causes self poisoning.[2]
[1] Proc. Natl. Acad. of Sci. USA, 2018, 115, 11680-11687.
[2] Phys. Chem. Chem. Phys., 2021, 23, 11345-11354.