A5 - 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 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

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), 12901297.

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 PlatinumRhodium 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), 23022308.

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), 874885.

DOI: 10.1021/acscatal.3c04337