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Boosting CO2 hydrogenation via size-dependent metal–support interactions in cobalt/ceria-based catalysts

DOI: 10.1038/s41929-020-0459-4 DOI Help

Authors: Alexander Parastaev (Eindhoven University of Technology) , Valerii Muravev (Eindhoven University of Technology) , Elisabet Huertas Osta (Eindhoven University of Technology) , Arno J. F. Van Hoof (Eindhoven University of Technology) , Tobias F. Kimpel (Eindhoven University of Technology) , Nikolay Kosinov (Eindhoven University of Technology) , Emiel J. M. Hensen (Eindhoven University of Technology)
Co-authored by industrial partner: No

Type: Journal Paper
Journal: Nature Catalysis , VOL 137

State: Published (Approved)
Published: May 2020
Diamond Proposal Number(s): 20715

Abstract: Metal–support interactions have a strong impact on the performance of heterogeneous catalysts. Specific sites at the metal–support interface can give rise to unusual high reactivity, and there is a growing interest in optimizing not only the properties of metal particles but also the metal–support interface. Here, we demonstrate how varying the particle size of the support (ceria–zirconia) can be used to tune the metal–support interactions, resulting in a substantially enhanced CO2 hydrogenation rate. A combination of X-ray diffraction, X-ray absorption spectroscopy, near-ambient pressure X-ray photoelectron spectroscopy, transmission electron microscopy and infrared spectroscopy provides insight into the active sites at the interface between cobalt and ceria–zirconia involved in CO2 hydrogenation to CH4. Reverse oxygen spillover from the support during treatment in hydrogen results in the generation of oxygen vacancies. Stabilization of cobalt particles by ceria–zirconia particles of intermediate size leads to oxygen spillover to the support during the CO2 and CO dissociation steps, followed by further hydrogenation of the resulting intermediates on cobalt.

Journal Keywords: Catalytic mechanisms; Chemical engineering; Heterogeneous catalysis; Nanoparticles

Subject Areas: Chemistry, Materials

Instruments: B18-Core EXAFS