Journal
APPLIED CATALYSIS B-ENVIRONMENTAL
Volume 162, Issue -, Pages 57-65Publisher
ELSEVIER SCIENCE BV
DOI: 10.1016/j.apcatb.2014.06.035
Keywords
CO2 hydrogenation; Dimethyl ether; Cu-ZnO-ZrO2 catalysts; Zeolites
Funding
- Italian Research Fund (PON R&C) through the BIO4BIO project, Biomolecular and Energy valorization of residual biomass from Agroindustry and Fishing Industry [DD 713/Ric. 29.10.2010, PON02_00451_3362376]
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A series of Cu-ZnO-ZrO2/H-ZSM5 multifunctional catalysts for the one-step CO2-to-DME hydrogenation reaction was prepared via coprecipitation of methanol catalyst precursors by means of different precipitating agents (i.e., sodium bicarbonate, ammonium carbonate, oxalic acid and urea) in a slurry containing dispersed zeolite particles. The samples were characterized by XRF, XRD, N-2 adsorption/desorption isotherms, SEM, N2O-titration, TPR and NH3/CO2 TPD techniques, while the catalytic testing was carried out in a fixed-bed reactor operating at 3.0 MPa, in the T-R range 473-513 K and space velocity of 10,000 h(-1) (CO2/H-2/N-2, 3/9/1). The experiments revealed that the preparation methodology significantly affects catalyst properties and hence catalyst activity. The multifunctional catalyst prepared via ammonium carbonate precipitation resulted to be the most active in CO2 conversion, also accomplishing high DME selectivity, with a maximum space-time yield of 0.225 kg(DME)/kg(cat)/h. Catalyst characterization disclosed that the strength of basic sites, the ratio between acid and basic sites along with the Cu particle sizes are crucial to achieve maximum catalytic performance, keeping CO selectivity to a minimum value. (C) 2014 Elsevier B.V. All rights reserved.
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