Selective gas adsorption and unique structural topology of a highly stable guest-free zeolite-type MOF material with N-rich chiral open channels

Selective gas adsorption and unique structural topology of a highly stable guest-free zeolite-type MOF material with N-rich chiral open channels
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具有富氮手性开放通道的高度稳定的无客体沸石型 MOF 材料的选择性气体吸附和独特的结构拓扑

DOI:
10.1002/chem.200701447
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发表时间:
2008-01-01
影响因子:
4.3
通讯作者:
Kitagawa, Susumu
Kitagawa, Susumu
中科院分区:
化学2区
文献类型:
--
作者:
Li, Jian-Rong;Tao, Ying;Kitagawa, Susumu

文献摘要

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设计并合成了一种新型多功能二位四唑盐配体2,3-二-1H-四唑-5-基吡嗪(H(2)dtp)。该配体与ZnCl2发生溶剂热反应,得到坚固的无客体三维类沸石手性金属有机骨架(MOF)配合物[Zn(dtp)],其在手性空间群P6(1)中结晶,并具有富氮壁的手性开放通道,直径约为4.1埃。该框架呈现出独特的均匀etd (8,3) 拓扑结构,是MOF 中该类型的第一个例子,并表现出高热稳定性,分解温度高于380 摄氏度和永久孔隙率。有趣的是,这种材料能够选择性地吸附 O-2 和 CO2 而不是 N-2 气体,这是 MOB 中的一个很好的例子。此外,C2H2和MeOH吸附结果表明,尽管框架通道具有可提供氢键位点的富氮壁,但没有观察到客体分子与微孔表面之间的N中心点中心点H氢键效应。
A new multifunctional ditopic tetrazolate-based ligand, 2,3-di-1H-tetrazol-5-ylpyrazine (H(2)dtp) has been designed and synthesized. The solvothermal reaction of this ligand with ZnCl2 gave a robust guest-free three-dimensional zeolite-like chiral metal-organic framework (MOF) complex, [Zn(dtp)], which crystallized in chiral space group P6(1) and possessed chiral open channels with nitrogen-rich walls and the diameter of approximately 4.1 angstrom. This framework presents a unique uniform etd (8,3) topology, is the first example of its type in MOFs, and exhibits high thermal stability with the decomposition temperature above 380 degrees C and permanent porosity. It is interesting that this material is able to selectively adsorb O-2 and CO2 over N-2 gas, being a fare example in MOB. In addition, C2H2 and MeOH adsorption results show that although the framework channel holds nitrogen-rich walls that may provide H-bonding sites, no N center dot center dot center dot H H-bond effect between the guest molecules and microporous surface was observed.