A1 - Structure and Chemical Reactivity of Size-Selected Clusters in Gas Phase
Objective
Project A1 aims to unravel the influence of size, structure, charge and oxidation state on the oxidation kinetics of CO, NO and CH4 adsorbates on ionic Ptn and Pdn (n<100) clusters and their alloys over a large temperature and partial pressure range. To this end we will use a unique combination of structure sensitive methods (TIED, IRPD) and reactivity measurements (RITMS) in gas-phase.
Together with ab initio computations these experiments will help to infer the intrinsic structural and electronic origins for catalytic activity. These insights will allow disentangling support effects from intrinsic properties and can help to control and tune the cluster support interaction for a given reaction.
Project-related publications by participating researchers
| Prof. Dr. Ueli Heiz |
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J. Eckhard, D. Neuwirth, M. Tschurl, U. Heiz, From oxidative degradation to direct oxidation: Size regimes in the consecutive reaction of cationic tantalum clusters with dioxygen. Phys. Chem. Chem. Phys. 2017, 19, 10863-10869 DOI: 10.1039/C7CP01293D |
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D. Neuwirth, J. Eckhard, B. Visser, M. Tschurl, U. Heiz, Two reaction regimes in the oxidation of larger cationic tantalum clusters (Tan+, n = 13–40) under multi-collision conditions. Phys. Chem. Chem. Phys. 2016, 18, 8115-8119 DOI: 10.1039/C5CP07245J |
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A. Crampton, M. Rötzer, U. Landman, U. Heiz, Can support acidity predict sub-nanometer catalyst activity trends? ACS Catal. 2017, 7, 6738 |
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A. Crampton, M. Rötzer, F. Schweinberger, B. Yoon, U. Landman, U. Heiz, Controlling ethylene hydrogenation reactivity on Pt13 clusters by varying the stoichiometry of the amorphous silica support. Angew. Chem. Int. Ed. 2016, 55, 8953-8957 |
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A. Crampton, M. Rötzer, C. Ridge, F. Schweinberger, U. Heiz, B. Yoon, U. Landman, Structure sensitivity in the nonscalable regime explored via catalysed ethylene hydrogenation on supported platinum nanoclusters. Nat. Commun. 2016, 7, 10389 DOI: 10.1038/ncomms10389 |
| PD Detlef Schooss |
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T. Rapps, R. Ahlrichs, E. Waldt, M.M. Kappes, D. Schooss, On the structures of 55-atom transition-metal clusters and their relationship to the crystalline bulk. Angew. Chem. Int. Ed. 2013, 52, 6102 |
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D. Bumüller, A.-S. Hehn, E. Waldt, R. Ahlrichs, M. M. Kappes, D. Schooss, Ruthenium cluster structure change induced by hydrogen adsorption: Ru19–. J. Phys. Chem. C, 2017, 121, 10645-10652 |
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E. Waldt, R. Ahlrichs, M.M. Kappes, D. Schooss, Structures of medium‐sized ruthenium clusters: The octahedral Motif. ChemPhysChem, 2014, 15, 862-865 |
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E. Waldt, A.-S. Hehn, R. Ahlrichs, M. M. Kappes, D. Schooss, Structural evolution of small ruthenium cluster anions. J. Chem. Phys. 2015, 142, 024319 DOI: 10.1063/1.4905267 |
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S. Kohaut, T. Rapps, K. Fink, D. Schooss, Structural evolution of palladium clusters Pd55- - Pd147-: Transition to the bulk.J. Phys. Chem. A, 2019, 123, 51, 10940-10946 |