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Colloidal Defect-Free Silicalite-1 Single Crystals: Preparation, Structure Characterization, Adsorption, and Separation Properties for Alcohol/Water Mixtures
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: 0000-0003-4582-0902
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
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2015 (English)In: Langmuir, ISSN 0743-7463, E-ISSN 1520-5827, Vol. 31, no 30, p. 8488-8494Article in journal (Refereed) Published
Abstract [en]

In this work, colloidal silicalite-1 single crystals are for the first time synthesized using fluoride as mineralizing agent at near neutral pH. SEM, TEM, DLS, XRD, solid-state 29Si MAS NMR, and adsorption/desorption experiments using nitrogen, water, n-butanol, and ethanol as adsorbates were used to characterize the crystals. The single crystals have a platelike habit with a length of less than 170 nm and an aspect ratio (length/width) of about 1.2, and the thickness of the crystals is less than 40 nm. Compared with silicalite-1 crystals grown using hydroxide as mineralizing agent, the amount of structural defects in the lattice is significantly reduced and the hydrophobicity is increased. Membrane separation and adsorption results show that the synthesized defect-free crystals present high selectivity to alcohols from alcohol/water mixtures. The n-butanol/water adsorption selectivities were ca. 165 and 14 for the defect-free crystals and a reference sample containing defects, respectively, illustrating the improvement in n-butanol/water selectivity by eliminating the polar silanol defects.

Place, publisher, year, edition, pages
2015. Vol. 31, no 30, p. 8488-8494
National Category
Chemical Process Engineering Physical Chemistry
Research subject
Chemical Technology; Chemistry of Interfaces
Identifiers
URN: urn:nbn:se:ltu:diva-7846DOI: 10.1021/acs.langmuir.5b02520ISI: 000359278000034Scopus ID: 2-s2.0-84938674785Local ID: 64403f34-d43d-43de-9d6f-b5e17b81fbdcOAI: oai:DiVA.org:ltu-7846DiVA, id: diva2:980736
Note
Validerad; 2015; Nivå 2; 20150725 (magr)Available from: 2016-09-29 Created: 2016-09-29 Last updated: 2018-07-10Bibliographically 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
Luleå: 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: 2018-08-17Bibliographically approved

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Zhou, HanMouzon, JohanneFarzaneh, AmirfarrokhAntzutkin, OlegGrahn, MattiasHedlund, Jonas

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