乙炔
材料科学
吸附
吡嗪
乙烯
化学工程
气体分离
多孔性
选择性
聚合物
选择性吸附
光圈(计算机存储器)
高分子化学
有机化学
复合材料
催化作用
化学
膜
物理
工程类
生物化学
声学
作者
Zheng Fang,Lidong Guo,Bixuan Gao,Liangying Li,Zhiguo Zhang,Qiwei Yang,Yiwen Yang,Baogen Su,Qilong Ren,Zongbi Bao
标识
DOI:10.1021/acsami.9b09231
摘要
The pore size of adsorbents plays a vital role in determining the overall separation performance of gas separation and purification by adsorption. In this work, the pore apertures of the coordination pillared layer (CPL) was systematically controlled by adjusting the length of pillared ligands. We used pyrazine, 4,4′-bipyridine, and 1,2-di(4-pyridyl)-ethylene with increased length to synthesize CPL-1 (L = pyrazine), CPL-2 (L = 4,4′-bipyridine), and CPL-5 [L = 1,2-di(4-pyridyl)-ethylene], respectively. The aperture size of these CPLs varies from 4 to 11 Å: CPL-1 (4 × 6 Å2), CPL-2 (9 × 6 Å2), and CPL-5 (11 × 6 Å2). Among the three frameworks, CPL-2 exhibits the highest C2H2 uptake at ambient conditions as it has moderate pore size and porosity. However, CPL-1 has the best separation performance in the breakthrough experiments with binary gas mixture of C2H2/C2H4, thanks to the optimal pore size nearly excluding C2H4, which is only observed in the state-of-the-art UTSA-300a so far. The DFT calculations were carried out to elucidate the specific adsorption sites for both acetylene and ethylene among these frameworks. The modeling results suggest that binding strength is highly related to aperture size and that CPL-1 shows the highest adsorption selectivity owing to the optimal pore size. This work demonstrates that engineering pore size enables us to fabricate the highly efficient metal–organic framework (MOF)-based adsorbents for specific gas separation on the basis of the isoreticular chemistry.
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