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Stuttgart 2012 – wissenschaftliches Programm

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MO: Fachverband Molekülphysik

MO 22: Cluster

MO 22.2: Vortrag

Freitag, 16. März 2012, 10:45–11:00, V38.02

(contribution withdrawn)

Structural Variability in Transition Metal Oxide Clusters: Gas Phase Vibrational Spectroscopy of V3O6−8+ — •Claudia Brieger1, Torsten Wende1, Jens Döbler2, Andrzej Niedziela2, Joachim Sauer2, Gerard Meijer1, and Knut R. Asmis11Fritz-Haber Institut der MPG, Berlin — 2Humboldt Universität Berlin

Vanadium oxides exhibit a high structural variability and redox activity which comes to play into heterogeneous catalysis. Interestingly, the structure of the active sites in vanadium oxide catalysts is often not well known. Infrared photodissociation (IRPD) spectroscopy can be used to obtain structural information on isolated clusters in the gas phase. Here, we study the structures of tri-nuclear vanadium oxide cations. IRPD spectra of V3O6+He1−4, V3O7+Ar0−1, and V3O8+Ar0−2 from 350 to 1200 cm−1 are presented. V3O7+ and V3O8+ have a cage-like structure whereas a chain isomer is found to be most stable for V3O6+. The binding of the rare gas atoms to V3O6−8+ clusters is found to be strong, up to 58 kJ/mol for Ar, and markedly isomer-dependent, resulting in two interesting effects. First, for V3O7+Ar1 and V3O8+Ar1 an energetic reordering of the isomers compared to the bare ion is observed, making the ring-motif the most stable one. Second, different isomers bind different number of rare gas atoms. We demonstrate, how both effects can be exploited to isolate and assign the contributions from multiple isomers to the IR spectrum. The present results exemplify the sensitivity of the structure of vanadium oxide clusters on small perturbations in their environment.

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