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Partially fluorinated MIL-47 and Al-MIL-53 frameworks: influence of functionalization on sorption and breathing properties

Shyam Prosad Biswas UGent, Tom Rémy, Sarah Couck, Dmitry Denysenko, Geert Rampelberg UGent, Joeri FM Denayer, Dirk Volkmer, Christophe Detavernier UGent and Pascal Van Der Voort UGent (2013) PHYSICAL CHEMISTRY CHEMICAL PHYSICS. 15(10). p.3552-3561
abstract
Two perfluorinated metal hydroxo terephthalates [M-III(OH)(BDC-F)]center dot n(guests) (M-III = V, MIL-47-F-AS or 1-AS; Al, Al-MIL-53-F-AS or 2-AS) (BDC-F = 2-fluoro-1,4-benzenedicarboxylate; AS = as-synthesized) have been synthesized by a hydrothermal method using microwave irradiation (1-AS) or conventional electric heating (2-AS), respectively. The unreacted or occluded H2BDC-F molecules can be removed under vacuum by direct thermal activation or exchange of guest molecules followed by thermal treatment leading to the empty-pore forms of the title compounds [V-IV(O)(BDC-F)] (MIL-47-F, 1) and [Al-III(OH)(BDC-F)] (Al-MIL-53-F, 2). Thermogravimetric analysis (TGA) and temperature-dependent XRPD (TDXRPD) experiments indicate that the compounds are stable up to 385 and 480 degrees C, respectively. Both of the thermally activated compounds exhibit significant microporosity, as verified by N-2, CO2, n-hexane, o- and p-xylene sorption analyses. The structural changes of 2 upon adsorption of CO2, n-hexane, o- and p-xylene were highly influenced due to functionalization by -F groups, as compared to parent Al-MIL-53. The -F groups also introduce a certain degree of hydrophobicity into the frameworks, as demonstrated by the H2O sorption analyses.
Please use this url to cite or link to this publication:
author
organization
year
type
journalArticle (original)
publication status
published
subject
keyword
GAS-ADSORPTION, CO2 ADSORPTION, ALUMINUM TEREPHTHALATE MIL-53, ADSORPTION PROPERTIES, METAL-ORGANIC FRAMEWORKS, DRUG-DELIVERY, SELECTIVE ADSORPTION, POWDER DIFFRACTION, XYLENE ISOMERS, SEPARATION
journal title
PHYSICAL CHEMISTRY CHEMICAL PHYSICS
Phys. Chem. Chem. Phys.
volume
15
issue
10
pages
3552 - 3561
Web of Science type
Article
Web of Science id
000314846600021
JCR category
PHYSICS, ATOMIC, MOLECULAR & CHEMICAL
JCR impact factor
4.198 (2013)
JCR rank
5/33 (2013)
JCR quartile
1 (2013)
ISSN
1463-9076
DOI
10.1039/c3cp44204g
project
GOA 01G00710
language
English
UGent publication?
yes
classification
A1
copyright statement
I have transferred the copyright for this publication to the publisher
id
3165969
handle
http://hdl.handle.net/1854/LU-3165969
date created
2013-03-15 14:13:11
date last changed
2018-01-29 12:11:52
@article{3165969,
  abstract     = {Two perfluorinated metal hydroxo terephthalates [M-III(OH)(BDC-F)]center dot n(guests) (M-III = V, MIL-47-F-AS or 1-AS; Al, Al-MIL-53-F-AS or 2-AS) (BDC-F = 2-fluoro-1,4-benzenedicarboxylate; AS = as-synthesized) have been synthesized by a hydrothermal method using microwave irradiation (1-AS) or conventional electric heating (2-AS), respectively. The unreacted or occluded H2BDC-F molecules can be removed under vacuum by direct thermal activation or exchange of guest molecules followed by thermal treatment leading to the empty-pore forms of the title compounds [V-IV(O)(BDC-F)] (MIL-47-F, 1) and [Al-III(OH)(BDC-F)] (Al-MIL-53-F, 2). Thermogravimetric analysis (TGA) and temperature-dependent XRPD (TDXRPD) experiments indicate that the compounds are stable up to 385 and 480 degrees C, respectively. Both of the thermally activated compounds exhibit significant microporosity, as verified by N-2, CO2, n-hexane, o- and p-xylene sorption analyses. The structural changes of 2 upon adsorption of CO2, n-hexane, o- and p-xylene were highly influenced due to functionalization by -F groups, as compared to parent Al-MIL-53. The -F groups also introduce a certain degree of hydrophobicity into the frameworks, as demonstrated by the H2O sorption analyses.},
  author       = {Biswas, Shyam Prosad and R{\'e}my, Tom and Couck, Sarah and Denysenko, Dmitry and Rampelberg, Geert and Denayer, Joeri FM and Volkmer, Dirk and Detavernier, Christophe and Van Der Voort, Pascal},
  issn         = {1463-9076},
  journal      = {PHYSICAL CHEMISTRY CHEMICAL PHYSICS},
  keyword      = {GAS-ADSORPTION,CO2 ADSORPTION,ALUMINUM TEREPHTHALATE MIL-53,ADSORPTION PROPERTIES,METAL-ORGANIC FRAMEWORKS,DRUG-DELIVERY,SELECTIVE ADSORPTION,POWDER DIFFRACTION,XYLENE ISOMERS,SEPARATION},
  language     = {eng},
  number       = {10},
  pages        = {3552--3561},
  title        = {Partially fluorinated MIL-47 and Al-MIL-53 frameworks: influence of functionalization on sorption and breathing properties},
  url          = {http://dx.doi.org/10.1039/c3cp44204g},
  volume       = {15},
  year         = {2013},
}

Chicago
Biswas, Shyam Prosad, Tom Rémy, Sarah Couck, Dmitry Denysenko, Geert Rampelberg, Joeri FM Denayer, Dirk Volkmer, Christophe Detavernier, and Pascal Van Der Voort. 2013. “Partially Fluorinated MIL-47 and Al-MIL-53 Frameworks: Influence of Functionalization on Sorption and Breathing Properties.” Physical Chemistry Chemical Physics 15 (10): 3552–3561.
APA
Biswas, S. P., Rémy, T., Couck, S., Denysenko, D., Rampelberg, G., Denayer, J. F., Volkmer, D., et al. (2013). Partially fluorinated MIL-47 and Al-MIL-53 frameworks: influence of functionalization on sorption and breathing properties. PHYSICAL CHEMISTRY CHEMICAL PHYSICS, 15(10), 3552–3561.
Vancouver
1.
Biswas SP, Rémy T, Couck S, Denysenko D, Rampelberg G, Denayer JF, et al. Partially fluorinated MIL-47 and Al-MIL-53 frameworks: influence of functionalization on sorption and breathing properties. PHYSICAL CHEMISTRY CHEMICAL PHYSICS. 2013;15(10):3552–61.
MLA
Biswas, Shyam Prosad, Tom Rémy, Sarah Couck, et al. “Partially Fluorinated MIL-47 and Al-MIL-53 Frameworks: Influence of Functionalization on Sorption and Breathing Properties.” PHYSICAL CHEMISTRY CHEMICAL PHYSICS 15.10 (2013): 3552–3561. Print.