A4 - Infrared Spectroscopy and Quantum Chemical Calculations on Oxide-Supported Metal Particles/Clusters

Objective

The goal of this project is a fundamental understanding of the active site of nanostructured metal/oxide catalysts based on a thorough surface science study combining experiment and theory on monocrystal model systems. We will focus on the spectroscopic characterization (polarization-dependent IRRAS and IR transmission in conjunction with XPS and NEXAFS) of oxide-supported Pt, Pd and PtPd nanoparticles under activation and reaction conditions. Structural information about the metal clusters in gas phase and deposited on TiO₂, CeO₂, and Al₂O₃ surfaces will be determined by a combined quantum chemical and experimental approach in cooperation with projects A1 and A2.

Project-related publications by participating researchers

Project- and subject-related list of publications
D. Bumüller, A. G. Yohannes, S. Kohaut, I. Kondov, M. M. Kappes, K. Fink, D. Schooss, Structures of Small Platinum Cluster Anions Pt_n^–: Experiment and Theory. J. Phys. Chem. A 2022, 126, 22, 3502–3510, DOI: 10.1021/acs.jpca.2c02142
L. Caulfield, E. Sauter, H. Idriss, Y. Wang, C. Wö ll, Bridging the Pressure and Materials Gap in Heterogeneous Catalysis: A Combined UHV, In Situ, and Operando Study Using Infrared Spectroscopy. J. Phys. Chem. C 2023, 127, 14023-14029, DOI: 10.1021/acs.jpcc.3c03567
S. Kohaut, T. Rapps, K. Fink, D. Schooss, Structural evolution of palladium clusters Pd₅₅^- - Pd₁₄₇^-:Transition to the bulk. J. Phys. Chem. A 2019, 123(51), 10940–10946, DOI: 10.1021/acs.jpca.9b093697507
S. Liu, Y. Li, X. Yu, S. Han, Y. Zhou, Y. Yang, H. Zhang, Z. Jiang, C. Zhu, W. Li, C. Wöll, Y. Wang, W. Shen, Tuning Crystal-Phase of Bimetallic Single-Nanoparticle for Catalytic Hydrogenation. Nature Commun. 2022, 13, 4559. DOI: 10.1038/s41467-022-32274-4
P. G. Lustemberg, P. N. Plessow, Y. Wang, C. Yang, A. Nefedov, F. Studt, C. Wöll, M. Verónica Ganduglia-Pirovano, Vibrational Frequencies of Cerium-Oxide-Bound CO: A Challenge for Conventional DFT Methods. Phys. Rev. Lett. 2020, 125, 256101. DOI: 10.1103/PhysRevLett.125.256101
F. Maurer, J. Jelic, J. J. Wang, A. Gänzler, P. Dolcet, C. Wöll, Y. Wang, F. Studt, M. Casapu, J.-D. Grunwaldt, Tracking the Formation, Fate and Consequence for Catalytic Activity of Pt Single Sites on CeO₂. Nature Catal. 2020, 3, 824-833, DOI: 10.1038/s41929-020-00508-7
J. Wang, Sauter, A. Nefedov, S. Heißler, F. Maurer, M. Casapu, J.-D. Grunwaldt, Y. Wang, C. Wöll, Dynamic Structural Evolution of Ceria-Supported Pt Particles: A Thorough Spectroscopic Study. J. Phys. Chem. C 2022, 126, 9051-9058. DOI: 10.1021/acs.jpcc.2c02420
C. Yang, M. Capdevila-Cortada, C. Dong, Y. Zhou, J. Wang, X. Yu, A. Nefedov, S. Heißler, N. López, W. Shen, C. Wöll, Y. Wang, Surface Refaceting Mechanism on Cubic Ceria. J. Phys. Chem. Lett. 2020, 11, 7925-7931. DOI: 10.1021/acs.jpclett.0c02409
A. G. Yohannes, K. Fink, I. Kondov, Pt nanoparticles under oxidizing conditions – implications of particle size, adsorption sites and oxygen coverage on stability. Nanoscale Adv. 2022, 4, 4554-4569. DOI: 10.1039/D2NA00490A
W. Xu, Y. Zhang, J. Wang, Y. Xu, L. Bian, Q. Ju, Y. Wang, Z. Fang, Defects Engineering Simultaneously Enhances Activity and Recyclability of MOFs in Selective Hydrogenation of Biomass. Nat. Commun. 2022, 13, 2068. DOI: 10.1038/s41467-022-29736-0

Project- and subject-related list of publications

D. Bumüller, A. G. Yohannes, S. Kohaut, I. Kondov, M. M. Kappes, K. Fink, D. Schooss, Structures of Small Platinum Cluster Anions Pt_n^–: Experiment and Theory. J. Phys. Chem. A 2022, 126, 22, 3502–3510,

DOI: 10.1021/acs.jpca.2c02142

L. Caulfield, E. Sauter, H. Idriss, Y. Wang, C. Wö ll, Bridging the Pressure and Materials Gap in Heterogeneous Catalysis: A Combined UHV, In Situ, and Operando Study Using Infrared Spectroscopy. J. Phys. Chem. C 2023, 127, 14023-14029,

DOI: 10.1021/acs.jpcc.3c03567

S. Kohaut, T. Rapps, K. Fink, D. Schooss, Structural evolution of palladium clusters Pd₅₅^- - Pd₁₄₇^-:Transition to the bulk. J. Phys. Chem. A 2019, 123(51), 10940–10946,

DOI: 10.1021/acs.jpca.9b093697507

S. Liu, Y. Li, X. Yu, S. Han, Y. Zhou, Y. Yang, H. Zhang, Z. Jiang, C. Zhu, W. Li, C. Wöll, Y. Wang, W. Shen, Tuning Crystal-Phase of Bimetallic Single-Nanoparticle for Catalytic Hydrogenation. Nature Commun. 2022, 13, 4559.

DOI: 10.1038/s41467-022-32274-4

P. G. Lustemberg, P. N. Plessow, Y. Wang, C. Yang, A. Nefedov, F. Studt, C. Wöll, M. Verónica Ganduglia-Pirovano, Vibrational Frequencies of Cerium-Oxide-Bound CO: A Challenge for Conventional DFT Methods. Phys. Rev. Lett. 2020, 125, 256101.

DOI: 10.1103/PhysRevLett.125.256101

F. Maurer, J. Jelic, J. J. Wang, A. Gänzler, P. Dolcet, C. Wöll, Y. Wang, F. Studt, M. Casapu, J.-D. Grunwaldt, Tracking the Formation, Fate and Consequence for Catalytic Activity of Pt Single Sites on CeO₂. Nature Catal. 2020, 3, 824-833,

DOI: 10.1038/s41929-020-00508-7

J. Wang, Sauter, A. Nefedov, S. Heißler, F. Maurer, M. Casapu, J.-D. Grunwaldt, Y. Wang, C. Wöll, Dynamic Structural Evolution of Ceria-Supported Pt Particles: A Thorough Spectroscopic Study. J. Phys. Chem. C 2022, 126, 9051-9058.

DOI: 10.1021/acs.jpcc.2c02420

C. Yang, M. Capdevila-Cortada, C. Dong, Y. Zhou, J. Wang, X. Yu, A. Nefedov, S. Heißler, N. López, W. Shen, C. Wöll, Y. Wang, Surface Refaceting Mechanism on Cubic Ceria. J. Phys. Chem. Lett. 2020, 11, 7925-7931.

DOI: 10.1021/acs.jpclett.0c02409

A. G. Yohannes, K. Fink, I. Kondov, Pt nanoparticles under oxidizing conditions – implications of particle size, adsorption sites and oxygen coverage on stability. Nanoscale Adv. 2022, 4, 4554-4569.

DOI: 10.1039/D2NA00490A

W. Xu, Y. Zhang, J. Wang, Y. Xu, L. Bian, Q. Ju, Y. Wang, Z. Fang, Defects Engineering Simultaneously Enhances Activity and Recyclability of MOFs in Selective Hydrogenation of Biomass. Nat. Commun. 2022, 13, 2068.

DOI: 10.1038/s41467-022-29736-0

Project Area A - Cluster & nano-particles