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Uptake of liquid alcohols by the flexible FeIII metal-organic framework MIL-53 observed by time-resolved in Situ X-ray diffraction
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Walton, Richard I., Munn, Alexis S., Guillou, Nathalie and Millange, Franck (2011) Uptake of liquid alcohols by the flexible FeIII metal-organic framework MIL-53 observed by time-resolved in Situ X-ray diffraction. Chemistry - A European Journal, Vol.17 (No.25). pp. 7069-7079. doi:10.1002/chem.201003634 ISSN 0947-6539.
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Official URL: http://dx.doi.org/10.1002/chem.201003634
Abstract
A comprehensive, time-resolved, energy-dispersive X-ray diffraction study of the uptake of liquid alcohols (methanol, ethanol, propan-1-ol and propan-2-ol) by the flexible metal-organic framework solid MIL-53(Fe)[H2O] is reported. In the case of the primary alcohols, a fluorinated version of the MIL-53(Fe) host (C2/c symmetry V ca. 1000 Å3), in which a fraction of framework hydroxides are replaced by fluoride, shows uptake of alcohols to give initially a partially expanded phase (C2/c symmetry, V ca. 1200 Å3) followed by an expanded form of the material (either Imcm or Pnam symmetry, V ca. 1600 Å3). In the case of methanol–water mixtures, the EDXRD data show that the partially open intermediate phase undergoes volume expansion during its existence, before switching to a fully open structure if concentrated methanol is used; analogous behaviour is seen if the initial guest is propan-2-ol, which then is replaced by pyridine, where a continuous shift of Bragg peaks within C2/c symmetry is observed. In contrast to the partially fluorinated materials, the purely hydroxylated host materials show little tendency to stabilise partially open forms of MIL-53(Fe) with primary alcohols and the kinetics of guest introduction are markedly slower without the framework fluorination: this is exemplified by the exchange of water by propan-2-ol, where a partially open C2/c phase is formed in a step-wise manner. Our study defines the various possible pathways of liquid-phase uptake of molecular guests by flexible solid MIL-53(Fe).
Item Type: | Journal Article | ||||
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Subjects: | Q Science > QD Chemistry | ||||
Divisions: | Faculty of Science, Engineering and Medicine > Science > Chemistry | ||||
Library of Congress Subject Headings (LCSH): | Organometallic chemistry, Solid state chemistry, X-rays -- Diffraction, Alcohols | ||||
Journal or Publication Title: | Chemistry - A European Journal | ||||
Publisher: | Wiley - V C H Verlag GmbH & Co. KGaA | ||||
ISSN: | 0947-6539 | ||||
Official Date: | 2011 | ||||
Dates: |
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Volume: | Vol.17 | ||||
Number: | No.25 | ||||
Page Range: | pp. 7069-7079 | ||||
DOI: | 10.1002/chem.201003634 | ||||
Status: | Peer Reviewed | ||||
Publication Status: | Published | ||||
Funder: | Seventh Framework Programme (European Commission) (FP7) | ||||
Grant number: | 228862 (FP7) |
Data sourced from Thomson Reuters' Web of Knowledge
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