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Instruments / Technical Area	Publication Details	Published	Actions
B18-Core EXAFS	Breaking structure sensitivity in CO2 hydrogenation by tuning metal–oxide interfaces in supported cobalt nanoparticles Alexander Parastaev , Valery Muravev , Elisabet Huertas Osta , Tobias F. Kimpel , Jérôme F. M. Simons , Arno J. F. Van Hoof , Evgeny Uslamin , Long Zhang , Job J. C. Struijs , Dudari B. Burueva , Ekaterina V. Pokochueva , Kirill V. Kovtunov , Igor V. Koptyug , Ignacio J. Villar-Garcia , Carlos Escudero , Thomas Altantzis , Pei Liu , Armand Béché , Sara Bals , Nikolay Kosinov , Emiel J. M. Hensen Nature Catalysis 46 DOI: 10.1038/s41929-022-00874-4 Diamond Proposal Number(s): [20715] Show Abstract ▼ Abstract: A high dispersion of the active metal phase of transition metals on oxide supports is important when designing efficient heterogeneous catalysts. Besides nanoparticles, clusters and even single metal atoms can be attractive for a wide range of reactions. However, many industrially relevant catalytic transformations suffer from structure sensitivity, where reducing the size of the metal particles below a certain size substantially lowers catalytic performance. A case in point is the low activity of small cobalt nanoparticles in the hydrogenation of CO and CO2. Here we show how engineering of catalytic sites at the metal–oxide interface in cerium oxide–zirconium dioxide (ceria–zirconia)-supported cobalt can overcome this structure sensitivity. Few-atom cobalt clusters dispersed on 3 nm cobalt(II)-oxide particles stabilized by ceria–zirconia yielded a highly active CO2 methanation catalyst with a specific activity higher than that of larger particles under the same conditions.	Nov 2022
B18-Core EXAFS	Operando spectroscopy unveils the catalytic role of different palladium oxidation states in CO oxidation on Pd/CeO2 catalysts Valery Muravev , Jérôme F. M. Simons , Alexander Parastaev , Marcel A. Verheijen , Job J. C. Struijs , Nikolay Kosinov , Emiel Hensen Angewandte Chemie International Edition DOI: 10.1002/anie.202200434 Diamond Proposal Number(s): [22225] Open Access Show Abstract ▼ Abstract: Aiming at knowledge-driven design of novel metal-ceria catalysts for automotive exhaust abatement, current efforts mostly pertain to the synthesis and understanding of well-defined systems. In contrast, technical catalysts are often heterogenous in their metal speciation. Here, we unveiled rich structural dynamics of a conventional impregnated Pd/CeO2 catalyst during CO oxidation. In situ X-ray photoelectron spectroscopy and operando X-ray absorption spectroscopy revealed presence of metallic and oxidic Pd states during the reaction. Using transient operando infrared spectroscopy, we probed the nature and reactivity of the surface intermediates involved in CO oxidation. We found that while low-temperature activity is associated with sub-oxidized and interfacial Pd sites, the reaction at elevated temperatures involves metallic Pd. These results highlight the utility of the multi-technique operando approach for establishing structure-activity relationships of technical catalysts.	Mar 2022

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