Pore chemistry and size control in hybrid porous materials for acetylene capture from ethylene
Pore chemistry and size control in hybrid porous materials for acetylene capture from ethylene
复制标题
用于从乙烯中捕获乙炔的杂化多孔材料的孔化学和尺寸控制
DOI：
10.1126/science.aaf2458
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发表时间：
2016-07-08
期刊：
影响因子：
56.9
通讯作者：
Chen, Banglin
中科院分区：
文献类型：
--
作者：
Cui, Xili;Chen, Kaijie;Chen, Banglin
将一种有机分子与另一种有机分子分离是一项挑战(见林的观点)。在高纯度聚合物生产中，需要将乙炔从乙烯中分离出来。崔等人。开发了一种含六氟硅酸盐和有机连接物的铜基金属-有机骨架，旨在对乙炔具有高亲和力。这些材料在每个孔中捕获四个乙炔分子，成功地将乙炔从与乙烯的混合物中分离出来。丙烷和丙烯都是重要的原料化学品。然而，它们在物理和化学上的相似性需要高能量的过程才能将它们分开。Cadiau等人。设计了一种氟化多孔金属-有机骨架材料，选择性地吸附丙烯，完全排除丙烷。科学，这一期，第141和137页；另见第121页。带有六氟硅酸盐连接体的铜基金属-有机骨架可以将乙炔从乙烯中分离出来。多孔材料的物理吸附能力和选择性之间的权衡是通过物理吸附有效分离和提纯气体的主要障碍。我们报道了六氟硅酸盐和有机连接物对金属配位网络中孔化学和大小的控制，目的是通过合作的主客体和/或客体相互作用来优先结合和有序组装乙炔分子。通过模拟和中子粉末衍射研究，验证了乙炔的特定结合部位。在环境条件下，与这些结合作用相关的能量为乙炔提供了高的吸附容量(0.025巴时为每克2.1毫米分子)和选择性(39.7至44.8.它们对乙炔/乙烯混合物的分离效率由实验穿透曲线(1/99混合物中每克0.73毫米分子)证明。
Separating one organic from another Separating closely related organic molecules is a challenge (see the Perspective by Lin).The separation of acetylene from ethylene is needed in high-purity polymer production. Cui et al. developed a copper-based metal-organic framework with hexafluorosilicate and organic linkers designed to have a high affinity for acetylene. These materials, which capture four acetylene molecules in each pore, successfully separated acetylene from mixtures with ethylene. Propane and propylene are both important feedstock chemicals. Their physical and chemical similarity, however, requires energy-intense processes to separate them. Cadiau et al. designed a fluorinated porous metal-organic framework material that selectively adsorbed propylene, with the complete exclusion of propane. Science, this issue pp. 141 and 137; see also p. 121 A copper-based metal-organic framework with hexafluorosilicate linkers can separate acetylene from ethylene. The trade-off between physical adsorption capacity and selectivity of porous materials is a major barrier for efficient gas separation and purification through physisorption. We report control over pore chemistry and size in metal coordination networks with hexafluorosilicate and organic linkers for the purpose of preferential binding and orderly assembly of acetylene molecules through cooperative host-guest and/or guest-guest interactions. The specific binding sites for acetylene are validated by modeling and neutron powder diffraction studies. The energies associated with these binding interactions afford high adsorption capacity (2.1 millimoles per gram at 0.025 bar) and selectivity (39.7 to 44.8) for acetylene at ambient conditions. Their efficiency for the separation of acetylene/ethylene mixtures is demonstrated by experimental breakthrough curves (0.73 millimoles per gram from a 1/99 mixture).