Hyper-Cross-linked Porous Organic Frameworks with Ultramicropores for Selective Xenon Capture

Hyper-Cross-linked Porous Organic Frameworks with Ultramicropores for Selective Xenon Capture
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DOI:
10.1021/acsami.9b01619
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发表时间:
2019-04-10
影响因子:
9.5
通讯作者:
Vaidhyanathan, Ramanathan
Vaidhyanathan, Ramanathan
中科院分区:
材料科学2区
文献类型:
--
作者:
Chakraborty, Debanjan;Nandi, Shyamapada;Vaidhyanathan, Ramanathan

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利用简单的Friedel-Crafts反应制备了具有超微孔结构的C-C键合多孔有机骨架材料(IISERP-POF 6,7,8)。这些聚合物表现出永久多孔性,Brunauer-Emmett-Teller表面积为645-800 m2/g。在298 K和1 bar的压力下,这些聚合物表现出选择性捕集能力(S(Kr/Kr)= 6.7,6.3和6.3)。有趣的是,对于1:99的Xe-N-2/Xe-CO2组成,这些聚合物还显示出显著的Xe/N-2(s(Xe/N-2)= 200、180和160,在298 K和1巴下)和Xe/CO2选择性(s(Xe/CO2)= 5.6、7.4和5.6)。在如此低的浓度下选择性地去除H2O是极其具有挑战性的;与在多孔碳和金属有机框架中观察到的那些相比,观察到的选择性更高。使用与核废气混合物相关的组合物与聚合物进行了突破性研究,并且我们发现聚合物在柱中保持时间更长,这说明了在动态条件下的Kr/Kr分离性能。
Exceptionally stable ultramicroporous C-C-bonded porous organic frameworks (IISERP-POF6, 7, 8) have been prepared using simple Friedel-Crafts reaction. These polymers exhibit permanent porosity with a Brunauer-Emmett-Teller surface area of 645-800 m(2)/g. Xe/Kr adsorptive separation has been carried out with these polymers, and they display selective Xe capture (s(Xe/Kr) = 6.7, 6.3, and 6.3) at 298 K and 1 bar pressure. Interestingly, these polymers also show remarkable Xe/N-2 (s(Xe/N-2) = 200, 180, and 160 at 298 K and 1 bar) and Xe/CO2 selectivity (s(Xe/CO2) = 5.6, 7.4, and 5.6) for a 1:99 composition of Xe-N-2/Xe-CO2. Selective removal of Xe at such low concentrations is extremely challenging; the observed selectivities are higher compared to those observed in porous carbons and metal-organic frameworks. Breakthrough studies were performed using the composition relevant to the nuclear off-gas mixture with the polymers, and we find that the polymers hold Xe for a longer time in the column, which illustrates the Xe/Kr separation performance under dynamic conditions.