A2 - Reactivity and Sintering of Size- and Composition-Selected Clusters on Supports

Objective

For better mechanistic understanding of atomic scale reaction mechanisms, we will apply mass-selective ion deposition of Ptx=1-80, Pdy=1-150 and PtxPdy onto oxide supports (CeO2, patterned graphene/CeO2, Si/SiO2, TiO2 and Al2O3). The clusters’ structural changes, size dispersion, sintering, reactivity and catalytic activity will be tracked under conditions approaching those of engine exhaust catalysis. Local probe (STM) and ensemble averaging (XPS, TDS, FT-IR, NAP-XPS) surface characterization will be correlated with MS-based probes of reactivity to study CO and NO oxidation, NO reduction by CO and CH4 oxidation.

Project-related publications by participating researchers

Project- and subject-related list of publications

A. Böttcher, R. Schwaiger, T. M. Pazdera, D. Exner, J. Hauns, D. Strelnikov, S. Lebedkin, R. Gröger, F. Esch, B.A.J. Lechner, M. M. Kappes, Nanoscale patterning at the Si/SiO2/graphene interface by focused He+ beam, Nanotechnology2020, 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

DOI: 10.1021/acscatal.1c01451

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

DOI: 10.1007/s11244-024-01920-0

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