Comparative Study of the Effect of Defects on Selective Adsorption of Butanol from Butanol/Water Binary Vapor Mixtures in Silicalite-1 Films

Farzaneh, Amirfarrokh; DeJaco, Robert F.; Ohlin, Lindsay; Holmgren, Allan; Siepmann, J. Ilja; Grahn, Mattias

doi:10.1021/acs.langmuir.7b02097

Title: Comparative Study of the Effect of Defects on Selective Adsorption of Butanol from Butanol/Water Binary Vapor Mixtures in Silicalite-1 Films

Journal Article · Wed Aug 02 00:00:00 EDT 2017 · Langmuir

DOI:https://doi.org/10.1021/acs.langmuir.7b02097· OSTI ID:1425198

Farzaneh, Amirfarrokh ^[1]; DeJaco, Robert F. ^[2]; Ohlin, Lindsay ^[1]; Holmgren, Allan ^[1];

^[2];

^[1]

Lulea Univ. of Technology, Lulea (Sweden). Chemical Technology
Univ. of Minnesota, Minneapolis, MN (United States). Dept. of Chemical Engineering and Materials Science and Dept. of Chemistry and Chemical Theory Center

A promising route for sustainable 1-butanol (butanol) production is ABE (acetone, butanol, ethanol) fermentation. However, recovery of the products is challenging because of the low concentrations obtained in the aqueous solution, thus hampering large-scale production of biobutanol. Membrane and adsorbent-based technologies using hydrophobic zeolites are interesting alternatives to traditional separation techniques (e.g., distillation) for energy-efficient separation of butanol from aqueous mixtures. To maximize the butanol over water selectivity of the material, it is important to reduce the number of hydrophilic adsorption sites. This can, for instance, be achieved by reducing the density of lattice defect sites where polar silanol groups are found. The density of silanol defects can be reduced by preparing the zeolite at neutral pH instead of using traditional synthesis solutions with high pH. In this work, binary adsorption of butanol and water in two silicalite-1 films was studied using in situ attenuated total reflectance–Fourier transform infrared (ATR-FTIR) spectroscopy under equal experimental conditions. One of the films was prepared in fluoride medium, whereas the other one was prepared at high pH using traditional synthesis conditions. The amounts of water and butanol adsorbed from binary vapor mixtures of varying composition were determined at 35 and 50 °C, and the corresponding adsorption selectivities were also obtained. Both samples showed very high selectivities (100–23 000) toward butanol under the conditions studied. The sample having low density of defects, in general, showed ca. a factor 10 times higher butanol selectivity than the sample having a higher density of defects at the same experimental conditions. This difference was due to a much lower adsorption of water in the sample with low density of internal defects. Analysis of molecular simulation trajectories provides insights on the local selectivities in the zeolite channel network and at the film surface.

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Research Organization:: Univ. of Delaware, Newark, DE (United States); Energy Frontier Research Centers (EFRC) (United States). Catalysis Center for Energy Innovation (CCEI)

Sponsoring Organization:: USDOE Office of Science (SC), Basic Energy Sciences (BES); Swedish Research Council (SRC)

Grant/Contract Number:: SC0001004; 2011-406

OSTI ID:: 1425198

Journal Information:: Langmuir, Vol. 33, Issue 34; ISSN 0743-7463

Publisher:: American Chemical SocietyCopyright Statement

Country of Publication:: United States

Language:: English

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Cited by: 20 works

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