A02 – Reactivity and Sintering of Size- and Composition-Selected Clusters on Supports

For a better mechanistic understanding of atomic scale reaction mechanisms, we will deposit mass-selected Ptx=1-80, Pdy=1-150 and PtxPdy onto single crystalline oxide supports (CeO2, TiO2 and SiO2). The clusters’ structural changes, size dispersion, sintering, reactivity and catalytic activity will be tracked under conditions approaching those of realistic emission control conditions. Using near-ambient pressure (NAP) methods, we perform scanning tunneling microscopy, (NAP-)STM, and X-ray photoelectron spectroscopy, (NAP-)XPS at pressures up to 25 mbar and correlate surface characterization with MS-based studies of reactivity to investigate CH4, NH3 and VOC oxidation.

Project-related publications by participating researchers

Project- and subject-related list of publications

A. Böttcher, R. Schwaiger, T. Pazdera, D. Exner, J. Hauns, D. Strelnikov, S. Lebedkin, R. Gröger, F. Esch, B.A.J. Lechner, M. Kappes, Nanoscale patterning at the Si/SiO2/graphene interface by focused He+ beam, Nanotechnology 2020, 31, 505302,

DOI: 10.1088/1361-6528/abb5cf.

P. Chakraborty, S. Malola, M. Neumaier, P. Weis, H. Häkkinen, M. Kappes, Elucidating the Structures of Intermediate Fragments during Stepwise Dissociation of Monolayer-Protected Silver Clusters, Angew. Chem. Int. Ed. 2023, 62, e2023058,

DOI: 10.1002/anie.202305836.

S. Kaiser, F. Maleki, K. Zhang, W. Harbich, U. Heiz, S. Tosoni, B.A.J. Lechner, G. Pacchioni, F. Esch, Cluster catalysis with lattice oxygen: tracing oxygen transport from a magnetite (001) support onto small Pt clusters. ACS Catal. 2021, 11, 9519-9529.

DOI: 10.1021/acs.jpcc.2c03851

S. Kaiser, J. Plansky, M. Krinninger, A. Shavorskiy, S. Zhu, U. Heiz, F. Esch, B.A.J. Lechner, Does Cluster Encapsulation Inhibit Sintering? Stabilization of Size-Selected Pt Clusters on Fe3O4(001) by SMSI, ACS Catalysis 2023, 13, 6203,

DOI: 10.1021/acscatal.3c00448.

M. Krinninger, N. Bock, S. Kaiser, J. Reich, T. Bruhm, F. Haag, F. Allegretti, U. Heiz, K. Köhler, B.A.J. Lechner, F. Esch, On-Surface Carbon Nitride Growth from Polymerization of 2,5,8-Triazido-s-heptazine, Chem. Mater. 2023, 35, 6762,

DOI: 10.1021/acs.chemmater.3c01030.

B.A.J. Lechner, F. Knoller, A. Bourgund, U. Heiz, F. Esch, A microscopy approach to investigating the energetics of small supported metal clusters. J. Phys. Chem. C 2018, 122, 22569-22576.

DOI: 10.1021/acs.jpcc.8b06866

P. Petzoldt, M. Eder, S. Mackewicz, M. Blum, T. Kratky, S. Günther, M. Tschurl, U. Heiz, B.A.J. Lechner, Tuning Strong Metal-Support Interaction Kinetics on Pt-Loaded TiO2(110) by Choosing the Pressure: A Combined Ultrahigh Vacuum/Near-Ambient Pressure XPS Study, J. Phys. Chem. C 2022, 126, 16127,

DOI: 10.1021/acs.jpcc.2c03851.

J. Reich, S. Kaiser, U. Heiz, J.-D. Grunwaldt, M. Kappes, F. Esch, B. A.J. Lechner, A critical view on the quantification of model catalyst activity, accepted for publication in Topics in Catalysis.

L. Xu, K.G. Papanikolaou, B.A.J. Lechner, L. Je, G.A. Somorjai, M. Salmeron, M. Mavrikakis, Formation of active sites on transition metals through reaction-driven migration of surface atoms. Science 2023, 380, 70-76.

DOI: 10.1126/science.add0089

B. Zugic, L. Wang, C. Heine, D.N. Zakharov, B.A.J. Lechner, E.A. Stach, J. Biener, M. Salmeron, R.J. Madix, C.M. Friend, Dynamic restructuring drives catalytic activity on nanoporous gold-silver alloy catalysts, Nat. Mater. 2017, 16, 558,

DOI: 10.1038/nmat4824

 

The project is funded since 2021 and is now in the second funding phase.