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group of Dalmon et al. [145,202–204]. Either commercial Pt-Sn/γ-Al2O3 [202], Pt-In/silicalite [145,203] or MFI supported Pt-In-Ge [204] catalysts placed in the core of the membrane tube were used. The effectiveness of the membrane reactor to improve dehydrogenation yields compared to the conventional reactor was up to four times higher [145]. When comparing mesoporous membranes with microporous zeolite membranes, the authors found hydrogen selectivity only for the latter, while the usage of larger-pored membranes led just to gas mixing at both sides of the membrane [202]. Moreover, the authors pointed on the importance of the precise control/selection of the operating parameters such as feed flow and sweep gas flow, as well as sweep gas configuration and found correlations between membrane reactor performance and membrane permeability or catalyst activity depending on the applied conditions [145,203]. In this regard, the reactor performance was limited by the catalyst activity under counter-current sweep flow conditions so that the catalyst was not active enough to follow the high membrane permeability. On the other side, choosing the co-current sweep configuration, the reactor performance was controlled by the membrane permeation efficiency and insufficient selectivity resulted thereby in reactants (i-butane) loss. Van Dyk et al. [204] confirmed these observations conducting a comparative study with microporous MFI and dense Pd membranes in membrane reactors packed with Pt-In-Ge/MFI catalyst. Generally, better yields were obtained with the membrane reactor configurations than with the conventional reactor. Nevertheless, the two membranes reached almost equal yields despite their different separation efficiencies so that the authors concluded that the membrane reactor performance was limited by the catalyst activity. At this point the fundamental work of Gokhale et al. [205] has to be mentioned. The authors presented insights on the relationship between permeation rates as function of separation selectivity and residence time. They focused on the possible operating conditions under which reactant loss controls conversion in dehydrogenation reactions. However, Illgen et al. [146] commented a feed dilution effect should always be considered during product analysis. It was stated that despite the high separation efficiency of the MFI zeolite membranes, e.g. a H2/i-butane mixture separation factor of 70 and a permeance of 1 m3/m2 h bar at the reaction temperature of 510 ◦C, the increased conversion up to 49% obtained in the PBMR at WHSV of 0.5 h−1, where the conversion of the conventional reactor was 29.1% was due to a great extent to the dilution of the reactant feed by the sweep gas and less to the removal of H2 from the reaction zone. Consequently, van den Bergh et al. [147] revealed the benefit of using small-pore zeolite DD3R membranes coupled to Cr2O3/Al2O3 catalysts in PBMR for the dehydrogenation of i-butane. The DD3R membrane is believed to be quite attractive for the present application since it is able to separate H2 and i-butane by molecular sieving effects. Accordingly, only H2 could pass the membrane and i-butane will be 24PDF Image | Zeolite Catalysis
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