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Adsorption of Butanol and Water Vapors in Silicalite‑1 Films with a Low Defect Density
Luleå University of Technology, Department of Civil, Environmental and Natural Resources Engineering, Chemical Engineering.
Luleå University of Technology, Department of Civil, Environmental and Natural Resources Engineering, Chemical Engineering.
Luleå University of Technology, Department of Civil, Environmental and Natural Resources Engineering, Chemical Engineering.ORCID iD: 0000-0003-1067-7990
Department of Materials and Environmental Chemistry, Stockholm University.
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Number of Authors: 7
2016 (English)In: Langmuir, ISSN 0743-7463, E-ISSN 1520-5827, Vol. 32, 11789-11798 p.Article in journal (Refereed) Published
Abstract [en]

Pure silica zeolites are potentially hydrophobic and have therefore been considered to be interesting candidates for separating alcohols, e.g., 1-butanol, from water. Zeolites are traditionally synthesized at high pH, leading to the formation of intracrystalline defects in the form of silanol defects in the framework. These silanol groups introduce polar adsorption sites into the framework, potentially reducing the adsorption selectivity toward alcohols in alcohol/water mixtures. In contrast, zeolites prepared at neutral pH using the fluoride route contain significantly fewer defects. Such crystals should show a much higher butanol/water selectivity than crystals prepared in traditional hydroxide (OH−) media. Moreover, silanol groups are present at the external surface of the zeolite crystals; therefore, minimizing the external surface of the studied adsorbent is important. In this work, we determine adsorption isotherms of 1-butanol and water in silicalite-1 films prepared in a fluoride (F−) medium using in situ attenuated total reflectance−Fourier transform infrared (ATR−FTIR) spectroscopy. This film was composed of well intergrown, plate-shaped b-oriented crystals, resulting in a low external area. Single-component adsorption isotherms of 1-butanol and water were determined in the temperature range of 35− 80 °C. The 1-butanol isotherms were typical for an adsorbate showing a high affinity for a microporous material and a large increase in the amount adsorbed at low partial pressures of 1-butanol. The Langmuir−Freundlich model was successfully fitted to the 1-butanol isotherms, and the heat of adsorption was determined. Water showed a very low affinity for the adsorbent, and the amounts adsorbed were very similar to previous reports for large silicalite-1 crystals prepared in a fluoride medium. The sample also adsorbed much less water than did a reference silicalite-1(OH−) film containing a high density of internal defects.The results show that silicalite-1 films prepared in a F− medium with a low density of defects and external area are very promising for the selective recovery of 1-butanol from aqueous solutions.

Place, publisher, year, edition, pages
2016. Vol. 32, 11789-11798 p.
National Category
Other Chemical Engineering Chemical Process Engineering
Research subject
Chemical Technology
Identifiers
URN: urn:nbn:se:ltu:diva-60688DOI: 10.1021/acs.langmuir.6b03326ISI: 000388156000009ScopusID: 2-s2.0-84995812342OAI: oai:DiVA.org:ltu-60688DiVA: diva2:1049609
Note

Validerad; 2016; Nivå 2; 2016-12-02 (andbra)

Available from: 2016-11-25 Created: 2016-11-25 Last updated: 2017-02-13Bibliographically approved
In thesis
1. Adsorption Properties of MFI-Type Zeolite Films for Upgrading of Biofuels
Open this publication in new window or tab >>Adsorption Properties of MFI-Type Zeolite Films for Upgrading of Biofuels
2016 (English)Doctoral thesis, comprehensive summary (Other academic)
Abstract [en]

With the depleting reservoirs of fossil fuels, increasing environmental concerns for flue-gas emissions from fossil-fuel combustion and growing world population, the need for the development of new sustainable fuels is higher than ever. However, to be able to compete with today’s mature technologies for production of fuels from fossil sources, new efficient processing alternatives for upgrading of biofuels must be developed.

   Bio-fuels produced by e.g. fermentative processes are promising alternatives to traditional chemicals and fuels produced from fossil sources. Recovery of biofuels by selective membranes and adsorbents has been identified as promising energy efficient recovery routes.

In this work, adsorption properties of MFI-type zeolite films were studied using in situ ATR-FTIR spectroscopy in order to understand the adsorption properties of these zeolites.

   Single component adsorption isotherms of butanol and water vapor were determined at different temperatures using ATR-FTIR spectroscopy. The Langmuir and Sips model were successfully fitted to experimental data, and the fitted parameters obtained in this work were in very good agreement with values reported in the literature. Adsorbed amounts of butanol and water from binary vapor mixtures were extracted from the infrared spectra as well as the adsorption selectivities. The silicalite-1 film prepared in fluoride medium found to be significantly more butanol selective due to the exceptionally low density of defects in the structure.

   Biogas (methane) is another promising biofuel that is commonly produced by anaerobic degradation of biomass. However, before it may be used, contaminants have to be removed from the gas; two of the most abundant contaminants in biogas are carbon dioxide and water vapor. Adsorption of a ternary mixture of methane, carbon dioxide and water vapor in zeolite Na-ZSM-5 has been studied at various compositions and temperatures using ATR–FTIR spectroscopy. The amount adsorbed determined from experimental data were compared to predictions by the Ideal Adsorbed Solution Theory (IAST). This result confirms that Na-ZSM-5 could be a promising membrane material for upgrading of biogas.

Place, publisher, year, edition, pages
Lluleå: Luleå University of Technology, 2016
National Category
Engineering and Technology Chemical Engineering
Research subject
Chemical Technology
Identifiers
urn:nbn:se:ltu:diva-60958 (URN)978-91-7583-781-9 (ISBN)978-91-7583-782-6 (ISBN)
Public defence
2017-02-20, C305, Luleå tekniska universitet, 10:00
Opponent
Supervisors
Available from: 2016-12-09 Created: 2016-12-07 Last updated: 2017-05-19Bibliographically approved

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