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A synthetic route to ultralight hierarchically micro/mesoporous Al(III)-carboxylate metal-organic aerogels.

Li L, Xiang S, Cao S, Zhang J, Ouyang G, Chen L, Su CY - Nat Commun (2013)

Bottom Line: Developing a synthetic methodology for the fabrication of hierarchically porous metal-organic monoliths that feature high surface area, low density and tunable porosity is imperative for mass transfer applications, including bulky molecule capture, heterogeneous catalysis and drug delivery.Heating represents a key factor in the control of gelation versus crystallization of Al(III)-multicarboxylate systems.The porosity of the resulting metal-organic aerogels can be readily tuned, leading to the formation of well-ordered intraparticle micropores and aerogel-specific interparticle mesopores, thereby integrating the merits of both crystalline metal-organic frameworks and light aerogels.

View Article: PubMed Central - PubMed

Affiliation: MOE Laboratory of Bioinorganic and Synthetic Chemistry, State Key Laboratory of Optoelectronic Materials and Technologies, Lehn Institute of Functional Materials, School of Chemistry and Chemical Engineering, Sun Yat-Sen University, Guangzhou 510275, China.

ABSTRACT
Developing a synthetic methodology for the fabrication of hierarchically porous metal-organic monoliths that feature high surface area, low density and tunable porosity is imperative for mass transfer applications, including bulky molecule capture, heterogeneous catalysis and drug delivery. Here we report a versatile and facile synthetic route towards ultralight micro/mesoporous metal-organic aerogels based on the two-step gelation of metal-organic framework nanoparticles. Heating represents a key factor in the control of gelation versus crystallization of Al(III)-multicarboxylate systems. The porosity of the resulting metal-organic aerogels can be readily tuned, leading to the formation of well-ordered intraparticle micropores and aerogel-specific interparticle mesopores, thereby integrating the merits of both crystalline metal-organic frameworks and light aerogels. The hierarchical micro/mesoporosity of the Al-metal-organic aerogels is thoroughly evaluated by N₂ sorption. The good accessibility of the micro/mesopores is verified by vapour/dye uptake, and their potential for utilization as effective fibre-coating absorbents is tested in solid-phase microextraction analyses.

No MeSH data available.


Related in: MedlinePlus

Dye uptake and SPEM data.(a) The kinetic curves of the AlBDC-3:2-0.15 MOA (7.5 mg) in 50 ml of dyes solution (100 mg l−1) for congo red (circle) and brilliant blue R-250 (square). The inserts show pictures of the dye-polluted water (I, III) before and (II, IV) after dye adsorption. (b) A schematic demonstration of the SPME analyses of a volatile analyte using the MOA-coated fibres (SEM image). (c) The extraction contrast profiles with AlBTC-3:2-0.05 MOA-coated and PDMS fibres for 1 ppm BTEX compounds. (d) The extraction contrast profiles with AlBTC-3:2-0.05 MOA-coated and PA fibres for 1 ppm phenols. The conditions for BTEX: extraction temperature, 298 K; extraction time, 10 min (stirring); desorption time, 0.5 min. PDMS, polydimethylsiloxane; B, benzene; T, toluene; E, ethylbenzene; X, xylene. Conditions for phenols: extraction temperature, 298 K; extraction time, 20 min (stirring); desorption time, 1 min. PA, polyacrylate; C, 2-chlorophenol; M, 4-methylphenol; N, 2-nitrophenol; D, 2,4-dichlorophenol; T, 2,4,6-trichlorophenol.
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f5: Dye uptake and SPEM data.(a) The kinetic curves of the AlBDC-3:2-0.15 MOA (7.5 mg) in 50 ml of dyes solution (100 mg l−1) for congo red (circle) and brilliant blue R-250 (square). The inserts show pictures of the dye-polluted water (I, III) before and (II, IV) after dye adsorption. (b) A schematic demonstration of the SPME analyses of a volatile analyte using the MOA-coated fibres (SEM image). (c) The extraction contrast profiles with AlBTC-3:2-0.05 MOA-coated and PDMS fibres for 1 ppm BTEX compounds. (d) The extraction contrast profiles with AlBTC-3:2-0.05 MOA-coated and PA fibres for 1 ppm phenols. The conditions for BTEX: extraction temperature, 298 K; extraction time, 10 min (stirring); desorption time, 0.5 min. PDMS, polydimethylsiloxane; B, benzene; T, toluene; E, ethylbenzene; X, xylene. Conditions for phenols: extraction temperature, 298 K; extraction time, 20 min (stirring); desorption time, 1 min. PA, polyacrylate; C, 2-chlorophenol; M, 4-methylphenol; N, 2-nitrophenol; D, 2,4-dichlorophenol; T, 2,4,6-trichlorophenol.

Mentions: To verify the accessibility of the MOAs for bulky molecule transportation, the aerogel AlBDC-3:2-0.15 was selected as a represented for the dye uptake test. The adsorption of congo red (CR) and brilliant blue R-250 (BBR-250) dyes was studied using UV–vis spectroscopy (Fig. 5a). The porous MOA displays a fast uptake of these dye molecules. Upon adsorption equilibrium, the high adsorbing capacities reach 633.4 and 621.3 mg g−1 for CR and BBR-250, respectively. This simply demonstrates that the mesopores of the MOAs are readily accessible to bulky organic molecules, which, in turn, may be able to facilitate interactions between the guests and micropores to enhance, for example, catalytic activity by nanoscale MOFPs.


A synthetic route to ultralight hierarchically micro/mesoporous Al(III)-carboxylate metal-organic aerogels.

Li L, Xiang S, Cao S, Zhang J, Ouyang G, Chen L, Su CY - Nat Commun (2013)

Dye uptake and SPEM data.(a) The kinetic curves of the AlBDC-3:2-0.15 MOA (7.5 mg) in 50 ml of dyes solution (100 mg l−1) for congo red (circle) and brilliant blue R-250 (square). The inserts show pictures of the dye-polluted water (I, III) before and (II, IV) after dye adsorption. (b) A schematic demonstration of the SPME analyses of a volatile analyte using the MOA-coated fibres (SEM image). (c) The extraction contrast profiles with AlBTC-3:2-0.05 MOA-coated and PDMS fibres for 1 ppm BTEX compounds. (d) The extraction contrast profiles with AlBTC-3:2-0.05 MOA-coated and PA fibres for 1 ppm phenols. The conditions for BTEX: extraction temperature, 298 K; extraction time, 10 min (stirring); desorption time, 0.5 min. PDMS, polydimethylsiloxane; B, benzene; T, toluene; E, ethylbenzene; X, xylene. Conditions for phenols: extraction temperature, 298 K; extraction time, 20 min (stirring); desorption time, 1 min. PA, polyacrylate; C, 2-chlorophenol; M, 4-methylphenol; N, 2-nitrophenol; D, 2,4-dichlorophenol; T, 2,4,6-trichlorophenol.
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Related In: Results  -  Collection

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f5: Dye uptake and SPEM data.(a) The kinetic curves of the AlBDC-3:2-0.15 MOA (7.5 mg) in 50 ml of dyes solution (100 mg l−1) for congo red (circle) and brilliant blue R-250 (square). The inserts show pictures of the dye-polluted water (I, III) before and (II, IV) after dye adsorption. (b) A schematic demonstration of the SPME analyses of a volatile analyte using the MOA-coated fibres (SEM image). (c) The extraction contrast profiles with AlBTC-3:2-0.05 MOA-coated and PDMS fibres for 1 ppm BTEX compounds. (d) The extraction contrast profiles with AlBTC-3:2-0.05 MOA-coated and PA fibres for 1 ppm phenols. The conditions for BTEX: extraction temperature, 298 K; extraction time, 10 min (stirring); desorption time, 0.5 min. PDMS, polydimethylsiloxane; B, benzene; T, toluene; E, ethylbenzene; X, xylene. Conditions for phenols: extraction temperature, 298 K; extraction time, 20 min (stirring); desorption time, 1 min. PA, polyacrylate; C, 2-chlorophenol; M, 4-methylphenol; N, 2-nitrophenol; D, 2,4-dichlorophenol; T, 2,4,6-trichlorophenol.
Mentions: To verify the accessibility of the MOAs for bulky molecule transportation, the aerogel AlBDC-3:2-0.15 was selected as a represented for the dye uptake test. The adsorption of congo red (CR) and brilliant blue R-250 (BBR-250) dyes was studied using UV–vis spectroscopy (Fig. 5a). The porous MOA displays a fast uptake of these dye molecules. Upon adsorption equilibrium, the high adsorbing capacities reach 633.4 and 621.3 mg g−1 for CR and BBR-250, respectively. This simply demonstrates that the mesopores of the MOAs are readily accessible to bulky organic molecules, which, in turn, may be able to facilitate interactions between the guests and micropores to enhance, for example, catalytic activity by nanoscale MOFPs.

Bottom Line: Developing a synthetic methodology for the fabrication of hierarchically porous metal-organic monoliths that feature high surface area, low density and tunable porosity is imperative for mass transfer applications, including bulky molecule capture, heterogeneous catalysis and drug delivery.Heating represents a key factor in the control of gelation versus crystallization of Al(III)-multicarboxylate systems.The porosity of the resulting metal-organic aerogels can be readily tuned, leading to the formation of well-ordered intraparticle micropores and aerogel-specific interparticle mesopores, thereby integrating the merits of both crystalline metal-organic frameworks and light aerogels.

View Article: PubMed Central - PubMed

Affiliation: MOE Laboratory of Bioinorganic and Synthetic Chemistry, State Key Laboratory of Optoelectronic Materials and Technologies, Lehn Institute of Functional Materials, School of Chemistry and Chemical Engineering, Sun Yat-Sen University, Guangzhou 510275, China.

ABSTRACT
Developing a synthetic methodology for the fabrication of hierarchically porous metal-organic monoliths that feature high surface area, low density and tunable porosity is imperative for mass transfer applications, including bulky molecule capture, heterogeneous catalysis and drug delivery. Here we report a versatile and facile synthetic route towards ultralight micro/mesoporous metal-organic aerogels based on the two-step gelation of metal-organic framework nanoparticles. Heating represents a key factor in the control of gelation versus crystallization of Al(III)-multicarboxylate systems. The porosity of the resulting metal-organic aerogels can be readily tuned, leading to the formation of well-ordered intraparticle micropores and aerogel-specific interparticle mesopores, thereby integrating the merits of both crystalline metal-organic frameworks and light aerogels. The hierarchical micro/mesoporosity of the Al-metal-organic aerogels is thoroughly evaluated by N₂ sorption. The good accessibility of the micro/mesopores is verified by vapour/dye uptake, and their potential for utilization as effective fibre-coating absorbents is tested in solid-phase microextraction analyses.

No MeSH data available.


Related in: MedlinePlus