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

(2013) PHYSICAL CHEMISTRY CHEMICAL PHYSICS. 15(10). p.3552-3561
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GOA 01G00710
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.
Keywords
GAS-ADSORPTION, CO2 ADSORPTION, ALUMINUM TEREPHTHALATE MIL-53, ADSORPTION PROPERTIES, METAL-ORGANIC FRAMEWORKS, DRUG-DELIVERY, SELECTIVE ADSORPTION, POWDER DIFFRACTION, XYLENE ISOMERS, SEPARATION

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Citation

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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.
@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},
}

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