Control of Pore Size and Functionality in Isoreticular Zeolitic Imidazolate Frameworks and their Carbon Dioxide Selective Capture Properties
Control of Pore Size and Functionality in Isoreticular Zeolitic Imidazolate Frameworks and their Carbon Dioxide Selective Capture Properties
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DOI：
10.1021/ja809459e
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发表时间：
2009-03-25
影响因子：
15
通讯作者：
Yaghi, Omar M.
中科院分区：
文献类型：
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作者：
Banerjee, Rahul;Furukawa, Hiroyasu;Yaghi, Omar M.
由硝酸锌(II)以及2-硝基咪唑和五种不同官能化咪唑的混合物制备了五种新的结晶沸石咪唑酯骨架(ZIF)，ZIF-78至-82，并发现它们具有GME拓扑结构。这些结构与之前报道的三种 GME ZIF 一起构成了一系列高孔隙率材料，其表面积为 620 至 1730 m(2)/g。孔径和孔径分别从7.1至15.9埃和3.8至13.1埃逐渐变化，装饰孔的官能团从极性氰基和硝基到非极性烷基变化。这些材料表现出的可变性使得它们作为气体分离介质的研究极具吸引力。计算出的 CO2 和 CH4 分离选择性值表明，具有 Potar 功能的 ZIF-ZIF-78 (10.6:1) 和 -82 (9.6:1) 比 GME 系列的其他成员和 BPL 活性炭能更大程度地保留 CO2 气体。这些预测在动态突破性研究中得到了证实，这些研究证实了 ZIF-78 和 -82 的容量增加，并证明了此类材料的前景。
Five new crystalline zeolitic imidazolate frameworks (ZIFs), ZIF-78 to -82, were prepared from zinc(II) nitrate and mixtures of 2-nitroimidazole and five different functionatized imidazoles and were found to have the GME topology. These structures, along with three previously reported GME ZIFs, constitute a series of highly porous materials with Brunauer-Emmet-Teller surface areas ranging from 620 to 1730 m(2)/g. The pore diameters and apertures vary incrementally from 7.1 to 15.9 angstrom and 3.8 to 13.1 angstrom, respectively, and the functionalities decorating the pores vary from polar cyano- and nitro- groups to nonpolar alkyl groups. The variability expressed in these materials makes them highly attractive for study as gas-separation media. Selectivity values calculated for separation of CO2 and CH4 predict that the ZIFs with potar functionatity, ZIF-78 (10.6: 1) and -82 (9.6: 1), retain CO2 gas to a greater degree than the other members of the GME series and BPL-activated carbon. These predictions are borne out in dynamic breakthrough studies, which confirm the increased capacity of ZIF-78 and -82 and demonstrate the promise of this class of materials.