期刊
CHEMISTRY-A EUROPEAN JOURNAL
卷 17, 期 18, 页码 5101-5109出版社
WILEY-BLACKWELL
DOI: 10.1002/chem.201002818
关键词
adsorption; functionalization; gas separation; gas storage; metal-organic framework
资金
- Department of Energy (DOE) [DE-FG02-08ER46491]
- U.S. Department of Energy (DOE) [DE-FG02-08ER46491] Funding Source: U.S. Department of Energy (DOE)
Hydroxyl-and amino-functionalized [Zn(BDC)(TED)(0.5)]center dot 2DMF center dot 0.2H(2)O leads to two new structures, [Zn(BDC-OH)(TED)(0.5)]center dot 1.5DMF center dot 0.3H(2)O and [Zn(BDC-NH(2))(TED)(0.5)]center dot xDMF center dot yH(2)O (BDC = terephthalic acid, TED = triethylenediamine, BDC-OH = 2-hydroxylterephthalic acid, BDC-NH(2) = 2-aminoterephthalic acid). Single-crystal Xray diffraction and powder X-ray diffraction studies confirmed that the structures of both functionalized compounds are very similar to that of their parent structure. Compound [Zn(BDC)(TED)(0.5)]center dot 2DMF center dot 0.2H(2)O can be considered a 3D porous structure with three interlacing 1D channels, whereas both [Zn(BDC-OH)-(TED)(0.5)]center dot 1.5DMF center dot 0.3H(2)O and [Zn(BDC-NH(2))(TED)(0.5)]center dot xDMF center dot yH(2)O contain only 1D open channels as a result of functionalization of the BDC ligand by the OH and NH(2) groups. A notable decrease in surface area and pore size is thus observed in both compounds. Consequently, [Zn(BDC)(TED)(0.5)]center dot 2DMF center dot 0.2H(2)O takes up the highest amount of H(2) at low temperatures. Interestingly, however, both [Zn(BDC-OH)(TED)(0.5)]center dot 1.5DMF center dot 0.3H(2)O and [Zn(BDC-NH(2))(TED)(0.5)]center dot xDMF center dot yH(2)O show significant enhancement in CO(2) uptake at room temperature, suggesting that the strong interactions between CO(2) and the functionalized ligands, indicating that surface chemistry, rather than porosity, plays a more important role in CO(2) adsorption. A comparison of single-component CO(2), CH(4), CO, N(2), and O(2) adsorption isotherms demonstrates that the adsorption selectivity of CO(2) over other small gases is considerably enhanced through functionalization of the frameworks. Infrared absorption spectroscopic measurements and theoretical calculations are also carried out to assess the effect of functional groups on CO(2) and H(2) adsorption potentials.
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