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Zeolite Catalysis

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Zeolite Catalysis ( zeolite-catalysis )

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temperature of only 450 ◦C a H2 volume content of 57 vol. % at a H2/CO ratio of 3.6 could be obtained from a methane/n-butane mixture with φC4H10 70.4 vol. % underlining the potential for natural gas processing and conversion. Considering product treatment, the membrane module is placed downstream to the catalytic reactor in order to purify the product stream, thus allowing membrane process conductions at operating conditions different from those of the catalytic unit. In this context, the applicability of zeolite membranes for the separation of hydrogen from reforming streams during syngas production has been recently reviewed [31,120]. Interestingly, during the evaluation of as-prepared and ion-exchanged zeolite LTA membranes for the separation of hydrogen from a simulated gas reformer mixtures, Cs-exchanged LTA membrane demonstrated stable H2 permeance in the presence of water [121]. Nenoff et al. evaluated theoretically the hydrogen separation selectivities of silicalite and ETS-10 membranes [122] as well as of zeolite NaA and zinc phosphate molecular sieve Na3ZnO(PO4)3 [123] using Grand Canonical Monte Carlo techniques. The same working group modified the internal surface of MFI-type zeolite membranes by silane precursors and obtained a H2/CO2 permselectivity of 141 combined with high hydrogen permeance [124]. On the other hand, the well-established capability of hydrophilic NaA zeolite membranes for selective water separation has entailed the first industrial implementation of zeolite membranes for de-watering of ethanol and i-propanol [43]. The high separation efficiency of this kind of membrane in pervaporation processes (see for instance reviews [13,125]) has motivated further research effort coupling water releasing reactions and water separations in equilibrium limited reactions. As an alternative to reactive distillation, different reactor configurations including pervaporation membranes could be applied in the esterification reactions [126], where the water permeation through the membrane is assisted by the mean of applied vacuum or sweep gas and then further condensed in a cold trap. In the last decades, membranes coupled to esterification processes have been investigated considering different zeolite structures, including zeolite A [127], sodalite (SOD) [128], chabazite CHA [129]. So for instance, Jafar et al. [127] investigated the homogeneously catalyzed esterification of lactic acid and ethanol by p-toluene sulphonic acid as catalyst, using a zeolite A membrane supported on carbon/zirconia tube for the separation of the produced water. Despite the superior performance of the zeolite A membrane in terms of water flux and selectivity [130,131], its low stability in acidic media [132] imposed the need of performing the process under vapor permeation conditions in order to avoid the direct contact of the membrane with the acidic reaction environment. Not surprisingly, high separation selectivities were achieved during the experiments resulting in significantly improved yields above the equilibrium limit. Similarly, Hasegawa et al. [129] adopted CHA-type zeolite membrane in the 11

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