A1 - Structure and Chemical Reactivity of Size-Selected Clusters in Gas Phase


Project A1 aims to unravel the influence of size, structure, charge and oxidation state on the oxidation kinetics of CO, NO and CHadsorbates 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

Project- and subject-related list of publications

D. Bumüller, A. G. Yohannes, S. Kohaut, I. Kondov, M. M. Kappes, K. Fink, D. Schooss, Structures of Small Platinum Cluster Anions Ptn: Experiment and Theory. J. Phys. Chem. A 2022, 126 (22), 3502-3510.

DOI: 10.1021/acs.jpca.2c02142

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 (20), 10645-10652.

DOI: 10.1021/acs.jpcc.6b09521

J. F. Eckhard, T. Masubuchi, M. Tschurl, R. N. Barnett, U. Landman, U. Heiz, Room-Temperature Methane Activation Mediated by Free Tantalum Cluster Cations: Size-by-Size Reactivity. J. Chem. Phys. A 2021, 125 (24), 5289-5302.

DOI: 10.1021/acs.jpca.1c02384

A.-S. Hehn, D. Bumüller, W. Klopper, M. M. Kappes, D. Schooss, Structural phase transition of ruthenium cluster hydrides. J. Phys. Chem. C 2020, 124 (26), 14306-14315.

DOI: 10.1021/acs.jpcc.0c01962

S. Kohaut, T. Rapps, K. Fink, D. Schooss, Structural evolution of palladium clusters Pd55Pd147: Transition to the bulk. J. Phys. Chem. A 2019, 123 (51), 10940-10946.

DOI: 10.1021/acs.jpca.9b09369

M. Kraft, J. R. Flores, W. Klopper, M. M. Kappes, D. Schooss, Structures of Small Tantalum Cluster Anions: Experiment and Theory. J. Phys. Chem. A 2021, 125 (15), 3135-3145.

DOI: 10.1021/acs.jpca.1c01250

J. Lengyel, N. Levin, F. J. Wensink, O. V. Lushchikova, R. N. Barnett, U. Landman, U. Heiz, J. M. Bakker, M. Tschurl, Carbide Dihydrides: Carbonaceous Species Identified in Ta4+-Mediated Methane Dehydrogenation. Angew. Chem. Int. Ed. 2020, 59 (52), 23631-23635.

DOI: 10.1002/anie.202010794

J. Lengyel, N. Levin, M. Ončák, K. Jakob, M. Tschurl, U. Heiz, Direct Coupling of Methane and Carbon Dioxide on Tantalum Cluster Cations. Chem. Eur. J. 2023, 29 (9), e202203259.

DOI: 10.1002/chem.202203259

T. Masubuchi, J. F. Eckhard, G. Goddard, M. Tschurl, U. Heiz, Thermal CO coupling reactions of Ta methylene clusters [TanCH2]+ (n = 1, 4) with O2. Phys. Chem. Chem. Phys. 2019, 21 (37), 20743-20749.

DOI: 10.1039/C9CP02739D

T. Masubuchi, J. F. Eckhard, K. Lange, B. Visser, M. Tschurl, U. Heiz, An efficient laser vaporization source for chemically modified metal clusters characterized by thermodynamics and kinetics. Rev. Sci. Instrum. 2018, 89 (2), 023104.

DOI: 10.1063/1.5017588