Synthesis, characterization and sorption properties of functionalized Cr-MIL-101-X (X=–F, –Cl, –Br, –CH{sub 3}, –C{sub 6}H{sub 4}, –F{sub 2}, –(CH{sub 3}){sub 2}) materials
- Department of Chemistry, Indian Institute of Technology Guwahati, 781039 Assam (India)
- Department of Chemical Engineering, Vrije Universiteit Brussel, Pleinlaan 2, 1050 Brussels (Belgium)
- Department of Inorganic and Physical Chemistry, Ghent University, COMOC – Center for Ordered Materials, Organometallics and Catalysis, Krijgslaan 281-S3, 9000 Ghent (Belgium)
Four existing and three new functionalized chromium terephthalates having MIL-101 topology and denoted as Cr-MIL-101-X (existing ones with X=–F, 1-F; –Cl, 2-Cl; –Br, 3-Br; –CH{sub 3}, 4-CH{sub 3}; new ones with X=–C{sub 6}H{sub 4}, 5-C{sub 6}H{sub 4}; –F{sub 2}, 6-F{sub 2}, –(CH{sub 3}){sub 2}, 7-(CH{sub 3}){sub 2}) were synthesized under hydrothermal conditions. All the materials except 5-C{sub 6}H{sub 4} could be prepared by a general synthetic route, in which the mixtures of CrO{sub 3}, H{sub 2}BDC-X (BDC=1,4-benzenedicarboxylate) linkers, conc. HCl and water with a molar ratio of 1:1:3.9:222.2 were reacted at 180 °C for 144 h. Compared to the 144 h of synthesis time, three of the compounds, namely 1-Cl, 2-Br and 5-C{sub 6}H{sub 4}, could be prepared in much shorter reaction times (12–18 h at 180–210 °C). The materials possess high thermal stability up to 270–300 °C in an air atmosphere. The activated compounds exhibit significant porosity (S{sub BET} range: 1273–2135 m{sup 2} g{sup −1}). At 0 °C and 1 bar, the CO{sub 2} adsorption capacities of the compounds fall in the 1.7–2.9 mmol g{sup −1} range. Compounds 1-F and 6-F{sub 2} showed enhanced CO{sub 2} uptake values compared to parent Cr-MIL-101. The benzene adsorption capacities of the compounds lie in the range of 66.2–139.5 molecules per unit cell at 50 °C and p/p{sub 0}=0.35. The increased benzene uptake value of 1-F compared to un-functionalized Cr-MIL-101 and 4-CH{sub 3} suggests that the fluorination has induced more hydrophobicity in Cr-MIL-101 as compared to the methylation. - Graphical abstract: Benzene adsorption by seven functionalized Cr-MIL-101-X metal-organic framework (MOF) materials Display Omitted - Highlights: • Seven functionalized Cr-MIL-101-X materials were synthesized solvothermally. • All Cr-MIL-101-X materials exhibited high thermal stability up to 270–300 °C in air. • All Cr-MIL-101-X compounds displayed considerable porosity towards N{sub 2}, CO{sub 2} and benzene. • Mono- and di-fluorinated Cr-MIL-101 materials showed enhanced CO{sub 2} adsorption capacities. • Cr-MIL-101-F adsorbed more benzene than non- and methyl-functionalized Cr-MIL-101.
- OSTI ID:
- 22584120
- Journal Information:
- Journal of Solid State Chemistry, Vol. 238; Other Information: Copyright (c) 2016 Elsevier Science B.V., Amsterdam, The Netherlands, All rights reserved.; Country of input: International Atomic Energy Agency (IAEA); ISSN 0022-4596
- Country of Publication:
- United States
- Language:
- English
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