Jan 31, 2013

Ligand functionalization and its effect on CO2 adsorption in microporous metal-organic frameworks

Chemistry, an Asian Journal
Hui LiuJing Li

Abstract

We report two new 3D structures, [Zn3(bpdc)3(2,2'-dmbpy)] (DMF)x(H2O)y (1) and [Zn3(bpdc)3(3,3'-dmbpy)]·(DMF)4(H2O)0.5 (2), by methyl functionalization of the pillar ligand in [Zn3(bpdc)3(bpy)] (DMF)4·(H2O) (3) (bpdc=biphenyl-4,4'-dicarboxylic acid; z,z'-dmbpy=z,z'-dimethyl-4,4'-bipyridine; bpy=4,4'-bipyridine). Single-crystal X-ray diffraction analysis indicates that 2 is isostructural to 3, and the power X-ray diffraction (PXRD) study shows a very similar framework of 1 to 2 and 3. Both 1 and 2 are 3D porous structures made of Zn3(COO)6 secondary building units (SBUs) and 2,2'- or 3,3'-dmbpy as pillar ligand. Thermogravimetric analysis (TGA) and PXRD studies reveal high thermal and water stability for both compounds. Gas-adsorption studies show that the reduction of surface area and pore volume by introducing a methyl group to the bpy ligand leads to a decrease in H2 uptake for both compounds. However, CO2 adsorption experiments with 1' (guest-free 1) indicate significant enhancement in CO2 uptake, whereas for 2' (guest-free 2) the adsorbed amount is decreased. These results suggest that there are two opposing and competitive effects brought on by methyl functionalization: the enhancement due to increased isosteric heats of C...Continue Reading

Mentioned in this Paper

Uptake
Dicarboxylic Acids
Adsorption
X-Ray Diffraction
Pore
Methyl Group
Diphenyl (fungicide)
Ligands Activity
4,4'-bipyridyl
Ligands

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