Journal
INDUSTRIAL & ENGINEERING CHEMISTRY RESEARCH
Volume 59, Issue 2, Pages 713-722Publisher
AMER CHEMICAL SOC
DOI: 10.1021/acs.iecr.9b05749
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Funding
- Ministry of Economy and Competitiveness of the Spanish Government [CTQ2016-77812-R]
- Basque Government [IT1218-19]
- ERDF funds
- European Commission [823745]
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The intensification of CO2 valorization has been theoretically studied in the direct synthesis of dimethyl ether (DME) carried out in a packed-bed reactor by means of two strategies pursuing the attenuation of the thermodynamic limitations of the process. Thus, the recycling of the nonconverted reactants, and the use of H2O perm-selective membranes, with different sweeping strategies has been studied. Special attention has been paid to improving the yield of DME and the conversion of CO2, seeking for a good balance between both objectives. The study has been conducted using the kinetic model previously established for a CuO-ZnO-MnO/SAPO-18 catalyst. Quantifying the deactivation kinetics in the kinetic model has allowed us to ascertain that both strategies contribute to attenuating deactivation. With a recirculation factor of 0.97, for a CO2/COx ratio in the feed of 0.25, at 275 degrees C and 30 bar, a CO2 conversion of 70% and a DME yield of 60% are achieved. Using in the simulation a membrane with a H2O permeability of 1 x 10(-7) mol s(-1) m(2) Pa-1 and a H2O/H-2 selectivity of 4, feasible with H-SOD type zeolite membranes, increases CO2 conversion up to 3.5-5% with regard to that obtained in a packed-bed reactor, and the upgrade in DME yield stands out, reaching an improvement of 25% for the hydrogenation of pure CO2, regardless of the sweeping strategy used (parallel or countercurrent mode, or the use of pure H-2 or H-2 + CO + CO2).
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