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Operando spectroscopy unveils the catalytic role of different palladium oxidation states in CO oxidation on Pd/CeO2 catalysts

DOI: 10.1002/anie.202200434 DOI Help

Authors: Valery Muravev (Technische Universiteit Eindhoven) , Jérôme F. M. Simons (Technische Universiteit Eindhoven) , Alexander Parastaev (Technische Universiteit Eindhoven) , Marcel A. Verheijen (Technische Universiteit Eindhoven) , Job J. C. Struijs (Technische Universiteit Eindhoven) , Nikolay Kosinov (Technische Universiteit Eindhoven) , Emiel Hensen (Technische Universiteit Eindhoven)
Co-authored by industrial partner: No

Type: Journal Paper
Journal: Angewandte Chemie International Edition

State: Published (Approved)
Published: March 2022
Diamond Proposal Number(s): 22225

Open Access Open Access

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.

Journal Keywords: operando DRIFTS; NAP-XPS; CO oxidation; ceria; structure-activity relationships

Subject Areas: Chemistry


Instruments: B18-Core EXAFS

Other Facilities: P65 at PETRA III, DESY

Added On: 25/03/2022 22:03

Documents:
Angew Chem Int Ed - 2022 - Muravev - Operando Spectroscopy Unveils the Catalytic Role of Different Palladium Oxidation.pdf

Discipline Tags:

Automotive Physical Chemistry Catalysis Chemistry Engineering & Technology

Technical Tags:

Spectroscopy X-ray Absorption Spectroscopy (XAS) Extended X-ray Absorption Fine Structure (EXAFS)