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Fine Tuning and Specific Binding Sites with a Porous Hydrogen-Bonded Metal-Complex Framework for Gas Selective Separations
Journal of the American Chemical Society ( IF 15.0 ) Pub Date : 2018-03-14 , DOI: 10.1021/jacs.7b13706
Zongbi Bao 1 , Danyan Xie 1 , Ganggang Chang 1, 2 , Hui Wu 3 , Liangying Li 1 , Wei Zhou 3 , Hailong Wang 4 , Zhiguo Zhang 1 , Huabin Xing 1 , Qiwei Yang 1 , Michael J. Zaworotko 5 , Qilong Ren 1 , Banglin Chen 4
Affiliation  

Research on hydrogen-bonded organic frameworks (HOFs) has been developed for quite a long time; however, those with both established permanent porosities and functional properties are extremely rare due to weak hydrogen-bonding interactions among molecular organic linkers, which are much more fragile and difficult to stabilize. Herein, through judiciously combining the superiority of both the moderately stable coordination bonds in metal-organic frameworks and hydrogen bonds, we have realized a microporous hydrogen-bonded metal-complex or metallotecton framework HOF-21, which not only shows permanent porosity, but also exhibits highly selective separation performance of C2H2/C2H4 at room temperature. The outstanding separation performance can be ascribed to sieving effect confined by the fine-tuning pores and the superimposed hydrogen-bonding interaction between C2H2 and SiF62- on both ends as validated by both modeling and neutron powder diffraction experiments. More importantly, the collapsed HOF-21 can be restored by simply immersing it into water or salt solution. To the best of our knowledge, such extraordinary water stability and restorability of HOF-21 were observed for the first time in HOFs, underlying the bright perspective of such new HOF materials for their industrial usage.

中文翻译:

用于气体选择性分离的多孔氢键金属复合骨架微调和特定结合位点

氢键有机骨架(HOFs)的研究已经发展了很长时间;然而,由于分子有机连接体之间的氢键相互作用较弱,这些分子有机连接体更加脆弱且难以稳定,因此具有既定永久孔隙率和功能特性的分子结构极为罕见。在此,通过明智地结合金属-有机骨架中适度稳定的配位键和氢键的优势,我们实现了一种微孔氢键金属配合物或金属构造骨架 HOF-21,它不仅显示出永久的孔隙率,而且在室温下表现出 C2H2/C2H4 的高选择性分离性能。出色的分离性能可归因于微调孔隙限制的筛分效应以及两端 C2H2 和 SiF62- 之间叠加的氢键相互作用,这通过建模和中子粉末衍射实验进行了验证。更重要的是,折叠的 HOF-21 可以通过简单地将其浸入水或盐溶液中来恢复。据我们所知,首次在 HOF 中观察到 HOF-21 的这种非凡的水稳定性和可恢复性,这为这种新型 HOF 材料在工业用途中的前景提供了基础。
更新日期:2018-03-14
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