Schering Stiftung

Preisträger*in 

Konrad Koszinowski

Schering Preis 2003

Konrad Koszinowski

Schering Preis 2003


Dr. Konrad Koszinowski vom Department of Chemistry, Stanford University, USA erhält den Schering Preis 2003 für seine Forschungsarbeit zu „Gaseous platinum clusters-versatile models for heterogeneous catalysts“.

„Gaseous platinum clusters-versatile models for heterogeneous catalysts“

Cationic platinum clusters are proposed as models for heterogeneous catalysts. In the gas-phase, the reactivity of the cluster ions can be thoroughly investigated by means of Fourier-transform ion-cyclotron-resonance mass spectrometry.

The reactions of Ptm+ clusters, m – 5, with several simple substrates exhibit distinct similarities to the analogous processes of heterogeneous catalysts. Encouraged by the thus demonstrated validity of the model approach chosen, methane activation by Ptm+ clusters is studied in detail. Kinetic isotope effects associated with dehydrogenation, hydrogen-deuterium exchange processes, and energy-dependent collision-induced dissociation experiments provide insight into the potential-energy surfaces of the surprisingly complex Ptm+/CH4 systems. The main difference between mononuclear platinum carbene PtCH2+ and the larger homologues PtmCH2+ concerns the interaction of carbon with more than a single metal center in the case of the clusters.

The resulting stronger platinum-carbon binding leads to a drastic change in reactivity. Instead of C-N coupling as observed for mononuclear PtCH2+, the clusters PtmCH2+ yield carbide complexes PtmC(NH3)+ upon reaction with ammonia. Whereas the first type of reactivity corresponds to the key step of the Degussa process for the large-scale synthesis of hydrogen cyanide from CH4 and NH3, the deviating behavior of the clusters can be considered as gas-phase analogue of undesired soot formation on the heterogeneous catalyst.

In the gas-phase model, reactivity can be controlled if bimetallic clusters are included. Unlike Pt2+, the heteronuclear cluster ions PtCu+, PtAg+, and PtAu+ efficiently mediate coupling of CH4 and NH3. On the basis of these results, the corresponding bimetallic catalysts are suggested for potential improvement of the Degussa process.

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