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Effect of alkali (Cs) doping on the surface chemistry and CO2 hydrogenation performance of CuO/CeO2 catalysts

Varvoutis Georgios, Lykaki Maria, Papista Eleni, Carabineiro, Sónia A. C, Psarras Antonios C., Marnellos Georgios E., Konsolakis Michail

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Extent12 pagesen
TitleEffect of alkali (Cs) doping on the surface chemistry and CO2 hydrogenation performance of CuO/CeO2 catalystsen
CreatorVarvoutis Georgiosen
CreatorLykaki Mariaen
CreatorΛυκακη Μαριαel
CreatorPapista Elenien
CreatorCarabineiro, Sónia A. Cen
CreatorPsarras Antonios C.en
CreatorMarnellos Georgios E.en
CreatorKonsolakis Michailen
CreatorΚονσολακης Μιχαηλel
Content SummaryThe reaction of captured carbon dioxide with renewable hydrogen towards the eventual indirect production of liquid hydrocarbons via CO2 reduction to CO (reverse water-gas shift reaction, rWGS) is a promising pathway in the general scheme of worldwide CO2 valorization. Copper-ceria oxides have been largely employed as rWGS catalysts owing to their unique properties linked to copper-ceria interactions. Here, we report on the fine-tuning of CuO/CeO2 composites by means of alkali promotion. In particular, this work aims at exploring the effect of cesium doping (0–4 atoms Cs per nm2) on co-precipitated CuO/CeO2 catalysts under CO2 hydrogenation conditions. The as-prepared samples were characterized by N2 physisorption, X-ray diffraction (XRD), H2-temperature programmed reduction (H2-TPR), X-ray photoelectron spectroscopy (XPS), CO2-temperature programmed desorption (CO2-TPD), Fourier-transform infrared spectroscopy (FTIR) of pyridine adsorption and CO-diffuse reflectance Fourier-transform infrared spectroscopy (CO-DRIFTS). The results demonstrated that a low amount of Cs exerted a beneficial effect on CO selectivity, inhibiting, however, CO2 conversion. Specifically, a doping of 2 atoms Cs per nm2 offers > 96 % CO selectivity and equilibrium CO2 conversion at temperatures as low as 430 °C, whereas further increase in cesium loading had no additional impact. The present findings can be mainly interpreted on a basis of the alkali effect on the textural and acid/base properties; Cs doping results in a significant reduction of the surface area and thus to a lower population of active sites for CO2 conversion, whereas it enhances the formation of basic sites and the stabilization of partially reduced Cu+ species, favoring CO selectivity.en
Type of ItemPeer-Reviewed Journal Publicationen
Type of ItemΔημοσίευση σε Περιοδικό με Κριτέςel
Date of Item2022-08-01-
Date of Publication2021-
SubjectCO hydrogenationen
SubjectReverse water-gas shift reactionen
SubjectCO Selectivityen
SubjectAlkali dopingen
SubjectCs promotionen
Bibliographic CitationG. Varvoutis, M. Lykaki, E. Papista, S. A. C. Carabineiro, A. C. Psarras, G. E. Marnellos, and M. Konsolakis, “Effect of alkali (Cs) doping on the surface chemistry and CO2 hydrogenation performance of CuO/CeO2 catalysts,” J. CO2 Util., vol. 44, Feb. 2021, doi: 10.1016/j.jcou.2020.101408.en