Carbon dioxide; Methanol to hydrocarbons; Paraffinic hydrocarbons; Proximity; Tandem catalyst; Zeolite; Bed configuration; Beta zeolite; Dual beds; Methanol-to-hydrocarbons; Silanols; Tandem system; ]+ catalyst; Environmental Chemistry; Chemistry (all); Chemical Engineering (all); Industrial and Manufacturing Engineering
Abstract :
[en] The tandem system for CO2 conversion to C4+ fuels through methanol as an intermediate, in one step, is studied in this work using ZnZrOx and beta zeolites. We show that the bed configuration is of major importance for such systems and highly dependent on the catalytic materials chosen. A dual bed configuration benefits the system showing the highest space time yield for C4+ paraffins when beta Si/Al = 15 is used (1.75 molC.kgcat−1.h−1) and an impressive selectivity of 40 % to isobutane. More beta zeolites with different Si/Al are tested in both mixed and dual bed configuration and correlations between the catalytic behavior and the acidic properties of the zeolites are made. A hypothesis on a correlation between the position of the hydroxy species, especially the silanols, and the difference in activity due to different proximities is proposed, as zeolites with more external silanols seem to benefit more from a dual bed configuration. Higher temperatures and GHSVs increase the production of paraffins but simultaneously increase CO selectivity. Moreover, the tandem system is found stable for more than 30 h. These results are essential for the further development of tandem catalytic systems converting CO2 to light alkanes.
Disciplines :
Chemical engineering
Author, co-author :
Lappa, Foteini ; Université de Liège - ULiège > Chemical engineering ; Center for Sustainable Catalysis and Engineering (CSCE), KU Leuven, Leuven, Belgium
Khalil, Ibrahim; Center for Sustainable Catalysis and Engineering (CSCE), KU Leuven, Leuven, Belgium ; Université Claude Bernard Lyon 1, CNRS, IRCELYON, Villeurbanne, France
Léonard, Grégoire ; Université de Liège - ULiège > Department of Chemical Engineering > PEPs - Products, Environment, and Processes
Dusselier, Michiel; Center for Sustainable Catalysis and Engineering (CSCE), KU Leuven, Leuven, Belgium
Language :
English
Title :
Bed configuration effects of tandem ZnZrOx-Beta zeolite catalysis in the one step methanol-mediated CO2 conversion to C4+ hydrocarbons
FWO - Fonds Wetenschappelijk Onderzoek Vlaanderen FPS Economy - Federal Public Service Economy KU Leuven - Catholic University of Leuven
Funding text :
F.L., G.L. and M. D. acknowledge the main funding for this work: BE-HyFE project funded by the federal Energy Transition Fund by FPS Economy. I.K. acknowledges the Research Foundation Flanders (FWO Vlaanderen) for the Senior postdoctoral research grant ( 12A3M24N ). M.D. acknowledges funding from KU Leuven grant C14/20/086 .
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