A5 - Structure and composition of PtPd model catalysts under operando conditions: experiment and simulation

Objective

The goal of this project is to elucidate active sites and deactivation mechanisms of Pt-Pd based model catalysts on Al₂O₃ and CeO₂ substrates with operando techniques during CO, methane as well as NO oxidation and reduction at the atomic scale. A combined experimental and theoretical approach will be pursued, unifying the most powerful methods such as surface sensitive X-ray diffraction in combination with mass spectrometry and kinetic Monte Carlo (kMC) simulations based on density functional theory. The shape and stability of Pt-Pd nanoparticles that is relevant for redispersion and sintering under operating conditions will be investigated by time resolved X-ray experiments and calculations.

Project-related publications by participating researchers

Dr. Philipp Pleßow
S. Zhang, P. N. Plessow, J. J. Willis, S. Dai, M. Xu, G. W. Graham, M. Cargnello, F. Abild-Pedersen, X. Pan, Dynamical observation and detailed description of catalysts under strong metal-support interaction, Nano Lett. 2016, 16, 4528-4534 DOI: 10.1021/acs.nanolett.6b01769
P. N. Plessow, F. Abild-Pedersen, Sintering of Pt nanoparticles via volatile PtO₂: Simulation and comparison with experiments, ACS Catal. 2016, 6, 7098-7108 DOI: 10.1021/acscatal.6b01646
E. M. Dietze, P. N. Plessow, Kinetic Monte Carlo model for gas phase diffusion in nanoscopic systems, J. Phys. Chem. C 2018, 122, 11524-11531 DOI: 10.1021/acs.jpcc.8b01816
E. D. Goodman, A. C. Johnston-Peck, E. M. Dietze, C. J. Wrasman, A. S. Hoffman, F. Abild-Pedersen, S. R. Bare, P. N. Plessow, M. Cargnello, Catalyst deactivation via decomposition into single atoms and the role of metal loading, Nat. Catal. 2019, 2, 748-755 DOI: 10.1038/s41929-019-0328-1
E. M. Dietze, P. N. Plessow, Predicting the strength of metal–support interaction with computational descriptors for adhesion energies, J. Phys. Chem. C, 2019, 123, 20443-20450 DOI: 10.1021/acs.jpcc.9b06893

Dr. Philipp Pleßow

S. Zhang, P. N. Plessow, J. J. Willis, S. Dai, M. Xu, G. W. Graham, M. Cargnello, F. Abild-Pedersen, X. Pan, Dynamical observation and detailed description of catalysts under strong metal-support interaction, Nano Lett. 2016, 16, 4528-4534

DOI: 10.1021/acs.nanolett.6b01769

P. N. Plessow, F. Abild-Pedersen, Sintering of Pt nanoparticles via volatile PtO₂: Simulation and comparison with experiments, ACS Catal. 2016, 6, 7098-7108

DOI: 10.1021/acscatal.6b01646

E. M. Dietze, P. N. Plessow, Kinetic Monte Carlo model for gas phase diffusion in nanoscopic systems, J. Phys. Chem. C 2018, 122, 11524-11531

DOI: 10.1021/acs.jpcc.8b01816

E. D. Goodman, A. C. Johnston-Peck, E. M. Dietze, C. J. Wrasman, A. S. Hoffman, F. Abild-Pedersen, S. R. Bare, P. N. Plessow, M. Cargnello, Catalyst deactivation via decomposition into single atoms and the role of metal loading, Nat. Catal. 2019, 2, 748-755

DOI: 10.1038/s41929-019-0328-1

E. M. Dietze, P. N. Plessow, Predicting the strength of metal–support interaction with computational descriptors for adhesion energies, J. Phys. Chem. C, 2019, 123, 20443-20450

DOI: 10.1021/acs.jpcc.9b06893

Prof. Dr. Andreas Stierle
J. Gustafson, M. Shipilin, C. Zhang, A. Stierle, U. Hejral, U. Ruett, O. Gutowski, P. A. Carlsson, M. Skoglundh, E. Lundgren, High-energy surface X-ray diffraction for fast surface structure determination, Science, 2014, 343, 758-751 DOI: 10.1126/science.1246834
Nolte, A. Stierle, N. Y. Jin-Phillipp, N. Kasper, T. U. Schulli, H. Dosch, Shape changes of supported Rh nanoparticles during oxidation and reduction cycles, Science, 2008, 321, 1654-1658 DOI: 10.1126/science.1160845
P. Nolte, A. Stierle, N. Kasper, N. Y. Jin-Phillipp, N. Jeutter, H. Dosch, Reversible shape changes of Pd nanoparticles on MgO (100), Nano Lett. 2011, 11, 4697-4700 DOI: 10.1021/nl2023564
U. Hejral, D. Franz, S. Volkov, S. Francoual, J. Strempfer, A. Stierle, Identification of a catalytically highly active surface phase for CO oxidation over PtRh nanoparticles under operando reaction conditions, Phys. Rev. Lett. 2018, 120, 126101 DOI: 10.1103/PhysRevLett.120.126101
U. Hejral, P. Müller, O. Balmes, D. Pontoni, A. Stierle, Tracking the shape-dependent sintering of platinum–rhodium model catalysts under operando conditions, Nat. Commun. 2016, 7, 10964 DOI: 10.1038/ncomms10964

Prof. Dr. Andreas Stierle

J. Gustafson, M. Shipilin, C. Zhang, A. Stierle, U. Hejral, U. Ruett, O. Gutowski, P. A. Carlsson, M. Skoglundh, E. Lundgren, High-energy surface X-ray diffraction for fast surface structure determination, Science, 2014, 343, 758-751

DOI: 10.1126/science.1246834

Nolte, A. Stierle, N. Y. Jin-Phillipp, N. Kasper, T. U. Schulli, H. Dosch, Shape changes of supported Rh nanoparticles during oxidation and reduction cycles, Science, 2008, 321, 1654-1658

DOI: 10.1126/science.1160845

P. Nolte, A. Stierle, N. Kasper, N. Y. Jin-Phillipp, N. Jeutter, H. Dosch, Reversible shape changes of Pd nanoparticles on MgO (100), Nano Lett. 2011, 11, 4697-4700

DOI: 10.1021/nl2023564

U. Hejral, D. Franz, S. Volkov, S. Francoual, J. Strempfer, A. Stierle, Identification of a catalytically highly active surface phase for CO oxidation over PtRh nanoparticles under operando reaction conditions, Phys. Rev. Lett. 2018, 120, 126101

DOI: 10.1103/PhysRevLett.120.126101

U. Hejral, P. Müller, O. Balmes, D. Pontoni, A. Stierle, Tracking the shape-dependent sintering of platinum–rhodium model catalysts under operando conditions, Nat. Commun. 2016, 7, 10964

DOI: 10.1038/ncomms10964

Project Area A - Cluster & nano-particles