A01 – Structure and Chemical Reactivity of Size-Selected Clusters in Gas Phase
The project aims to elucidate structure-reactivity relationships, reaction and deactivation mechanisms, and the role of different size regimes in the oxidation of NH3 and CH4 on ionic Ptn, Pdn and Run (n<100) clusters in gas phase. A unique combination of a structure sensitive method (TIED) and reactivity measurements (RITMS) under different reaction temperatures and reactant pressures will allow to unravel the origins of reactivity on an atomic scale. In this way, intrinsic cluster properties can be identified, analyzed by ab initio computations, and the reactivities compared to those of realistic systems.
The project is funded since 2021 and is now in the second funding phase.
Project-related publications by participating researchers
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Project- and subject-related list of publications |
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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. |
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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 (20), 10645-10652. DOI: 10.1021/acs.jpcc.6b09521. |
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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. |
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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. |
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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. DOI: 10.1021/acs.jpca.9b09369. |
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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. |
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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. |
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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. |
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T. Masubuchi, J. F. Eckhard, G. Goddard, M. Tschurl, U. Heiz, Thermal C–O 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. |
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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. |