A04 – Infrared Spectroscopy and Quantum Chemical Calculations on Oxide-Supported Metal Particles/Clusters

Project A04 focuses on a thorough surface science study on the adsorption and reactions of NH₃, CH₄, and VOCs on metal/oxide model systems by combining IR investigations and DFT calculations. We aim at a profound insight into the complex surface chemistry of noble metals (Pt, Pd, Ru) deposited on oxide nanoparticles (CeO₂, TiO₂, Al₂O₃) based on comprehensive reference data collected for single crystal systems. The structural and electronic properties of metal clusters in gas phase and on surfaces will be studied by quantum chemical methods. Furthermore, defects and dopants will be characterized by a combination of IRRAS and embedded cluster calculations.

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.

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

Project Area A - Cluster & nano-particles