A05 – Structure and Composition of PtPd Model Catalysts under operando Conditions: Experiment and Simulation

The goal of this project is to elucidate active sites and deactivation mechanisms of Pt-Pd, Rh and Ru based model catalysts on Al₂O₃ and CeO₂ substrates with in situ and operando techniques during methane as well as selective catalytic ammonia oxidation at the atomic scale. In the experimental and theoretical approach, most powerful methods such as in situ surface sensitive X-ray diffraction and kinetic Monte Carlo simulations based on density functional theory will be combined. The project will highlight the influence of support doping on activity and nanoparticle stability, as well as a comparison of structure – activity relations for steady state and transient light off conditions.

Project-related publications by participating researchers

Project- and subject-related list of publications
A. Aitbekova, C. Zhou, M. L. Stone, J. S. Lezama-Pacheco, A. C. Yang, A. S. Hoffman, E. D. Goodman, P. Huber, J. F. Stebbins, K. C. Bustillo, P. Ercius, J. Ciston, S. R. Bare, P. N. Plessow, M. Cargnello, Templated Encapsulation of Platinum-Based Catalysts Promotes High-Temperature Stability to 1,100 °C. Nat. Mater. 2022, 21 (11), 1290–1297. DOI: 10.1038/s41563-022-01376-1.
J. Chen, D. Sharapa, P. N. Plessow, Stability and Formation of Hydroxylated α-Al₂O₃(0001) Surfaces at High Temperatures. Phys. Rev. Res. 2022, 4 (1), 013232. DOI: 10.1103/PhysRevResearch.4.013232.
S. Chung, J.-C. Schober, S. Tober, D. Schmidt, A. Khadiev, D. V Novikov, V. Vonk, A. Stierle, Epitaxy and Shape Heterogeneity of a Nanoparticle Ensemble during Redox Cycles. ACS Nano 2021, 15 (8), 13267. DOI: 10.1021/acsnano.1c03002.
S. Dolling, CO Adsorption on PdPt Alloy Nanoparticles, Master thesis University of Hamburg 2022. DOI: 10.3204/PUBDB-2024-00899
U. Hejral, P. Plessow, D. Franz, M. Shipilin, O. Gutowski, U. Rütt, H. Noei, V. Vonk, A. Stierle, Composition-Dependent Alloy Nanoparticle Shape Changes under Reaction Conditions: Kinetic and Thermodynamic Effects, J. Phys. Chem. C 2024, DOI: 0.1021/acs.jpcc.4c00042.
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 (12), 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. Comm. 2016, 7 (1), 10964. DOI: 10.1038/ncomms10964.
Y. Y. Kim, T. F. Keller, T. J. Goncalves, M. Abuin, H. Runge, L. Gelisio, J. Carnis, V. Vonk, P. N. Plessow, I. A. Vartaniants, A. Stierle, Single Alloy Nanoparticle X-Ray Imaging during a Catalytic Reaction. Sci. Adv. 2021, 7 (40), eabh0757. DOI: 10.1126/sciadv.abh0757.
P. N. Plessow, C. T. Campbell, Influence of Adhesion on the Chemical Potential of Supported Nanoparticles as Modeled with Spherical Caps. ACS Catal. 2022, 12 (4), 2302–2308. DOI: 10.1021/acscatal.1c04633.
S. Saini, J. Halldin Stenlid, S. Deo, P. N. Plessow, F. Abild-Pedersen, A First-Principles Approach to Modeling Surface Site Stabilities on Multimetallic Catalysts. ACS Catal. 2024, 14 (2), 874–885. DOI: 10.1021/acscatal.3c04337.

Project- and subject-related list of publications

A. Aitbekova, C. Zhou, M. L. Stone, J. S. Lezama-Pacheco, A. C. Yang, A. S. Hoffman, E. D. Goodman, P. Huber, J. F. Stebbins, K. C. Bustillo, P. Ercius, J. Ciston, S. R. Bare, P. N. Plessow, M. Cargnello, Templated Encapsulation of Platinum-Based Catalysts Promotes High-Temperature Stability to 1,100 °C. Nat. Mater. 2022, 21 (11), 1290–1297.

DOI: 10.1038/s41563-022-01376-1.

J. Chen, D. Sharapa, P. N. Plessow, Stability and Formation of Hydroxylated α-Al₂O₃(0001) Surfaces at High Temperatures. Phys. Rev. Res. 2022, 4 (1), 013232.

DOI: 10.1103/PhysRevResearch.4.013232.

S. Chung, J.-C. Schober, S. Tober, D. Schmidt, A. Khadiev, D. V Novikov, V. Vonk, A. Stierle, Epitaxy and Shape Heterogeneity of a Nanoparticle Ensemble during Redox Cycles. ACS Nano 2021, 15 (8), 13267.

DOI: 10.1021/acsnano.1c03002.

S. Dolling, CO Adsorption on PdPt Alloy Nanoparticles, Master thesis University of Hamburg 2022.

DOI: 10.3204/PUBDB-2024-00899

U. Hejral, P. Plessow, D. Franz, M. Shipilin, O. Gutowski, U. Rütt, H. Noei, V. Vonk, A. Stierle, Composition-Dependent Alloy Nanoparticle Shape Changes under Reaction Conditions: Kinetic and Thermodynamic Effects, J. Phys. Chem. C 2024,

DOI: 0.1021/acs.jpcc.4c00042.

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 (12), 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. Comm. 2016, 7 (1), 10964.

DOI: 10.1038/ncomms10964.

Y. Y. Kim, T. F. Keller, T. J. Goncalves, M. Abuin, H. Runge, L. Gelisio, J. Carnis, V. Vonk, P. N. Plessow, I. A. Vartaniants, A. Stierle, Single Alloy Nanoparticle X-Ray Imaging during a Catalytic Reaction. Sci. Adv. 2021, 7 (40), eabh0757.

DOI: 10.1126/sciadv.abh0757.

P. N. Plessow, C. T. Campbell, Influence of Adhesion on the Chemical Potential of Supported Nanoparticles as Modeled with Spherical Caps. ACS Catal. 2022, 12 (4), 2302–2308.

DOI: 10.1021/acscatal.1c04633.

S. Saini, J. Halldin Stenlid, S. Deo, P. N. Plessow, F. Abild-Pedersen, A First-Principles Approach to Modeling Surface Site Stabilities on Multimetallic Catalysts. ACS Catal. 2024, 14 (2), 874–885.

DOI: 10.1021/acscatal.3c04337.

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

Project Area A - Cluster & nano-particles