Micro- and mesoporous supports for CO2 methanation catalysts: A comparison between SBA-15, MCM-41 and USY zeolite. (16th January 2018)

• Record Type: Journal Article
• Authors: Bacariza, M.C.; Graça, I.; Bebiano, S.S.; Lopes, J.M.; Henriques, C.
• Is Part Of: Chemical engineering science. Volume 175(2018)
• Page Start: 72
• Page End: 83
• Publication Date: 2018-01-16
• Subjects: SBA-15 -- MCM-41 -- Zeolite -- Nickel -- CO2 methanation -- FTIR Operando; Chemical engineering -- Periodicals; Génie chimique -- Périodiques; Chemical engineering; Periodicals; Electronic journals; 660
• DOI: 10.1016/j.ces.2017.09.027
• Languages: English
• ISSNs: 0009-2509

Abstract

Graphical abstract: Highlights: SBA-15 presented similar textural properties whatever the synthesis method used. Ni particles were mainly located on the SBA-15 and MCM-41 outer surfaces. Ni 0 dispersion was higher on SBA-15 and zeolite materials than on MCM-41. The highest TOFs and the lowest NiO band gap was obtained for 15%Ni/MCM-41. Improved activity was found when adding Ce due to the enhancement of CO2 activation. Abstract: Mesoporous SBA-15 synthesized by two different methods and MCM-41 were used as supports for Ni and Ni-Ce catalysts applied in CO2 methanation reaction. The performances obtained for both materials were compared taking into account the differences in terms of textural properties, Ni species and reaction mechanism. Results were compared with the reported in the literature for a microporous USY zeolite. XRD, DRS UV–Vis, H2 -TPR and TEM were used for the characterization of the samples. Catalytic tests were performed under the same conditions for all catalysts. Finally, FTIR Operando studies were carried out in order to establish differences from the mechanistically point of view as well as in terms of CO2 adsorption species for the different samples. Promising data was obtained with the Ni-based SBA-15 catalysts whatever the preparation method. Despite the greater Ni particles size, MCM-41 also reported interesting catalytic performances, so that presenting the highest TOF values among the catalysts studied. The good results obtained for the MCM-41 could be explained by the lower amount of non-reactive carbonyl species adsorbed on the Ni 0 particles surface during the reaction as well as by the enhanced interaction between metal and support reflected in the calculated band gap values. All the results are comparable to the obtained using a HNaUSY zeolite with Si/Al = 2.8 as support. Cerium incorporation on Ni/mesoporous supports allowed enhancing the CO2 conversion, especially at lower temperatures, as already reported for the zeolite-based samples.