A novel anion-pillared metal-organic framework for highly efficient separation of acetylene from ethylene and carbon dioxide†
A novel anion-pillared metal-organic framework for highly efficient separation of acetylene from ethylene and carbon dioxide†
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一种新型阴离子柱金属有机框架，用于高效分离乙炔与乙烯和二氧化碳
DOI：
10.1039/d0ta11340a
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发表时间：
2021-03-12
影响因子：
11.9
通讯作者：
Qian, Guodong
中科院分区：
文献类型：
--
作者：
Qian, Quan-Li;Gu, Xiao-Wen;Qian, Guodong
将乙炔 (C2H2) 与乙烯 (C2H4) 和二氧化碳 (CO2) 分离在石化工业中非常重要，但由于它们的尺寸和物理性质非常相似，因此仍然是一项艰巨的挑战。尽管许多多孔材料已被开发为用于 C2H2/C2H4 或 C2H2/CO2 分离的有前途的吸附剂，但很少有材料同时对两种气体混合物表现出高选择性。在此，我们报告了使用四连接的N-供体有机连接体构建了一种新型水稳定性SIFSIX型材料[Cu(TPB)SiF6](n)（称为ZJU-280，TPB = 1,2,4,5-四（吡啶-4-基）苯）。该材料具有合适的菱形孔和功能表面，可与 C2H2 分子实现最佳相互作用，在环境条件下提供高 C2H2 捕获能力，同时具有高 C2H2/CO2 (18.1) 和 C2H2/C2H4 (44.5) 选择性。理论计算表明，合适的菱形孔和功能位点可以提供多点结合环境，不仅可以优先与C2H2相互作用，而且可以使C2H2分子在框架内致密堆积。实际的突破性实验表明，ZJU-280a可以分别从C2H2/CO2（50/50，v/v）和C2H2/C2H4（1/99和50/50）混合物中有效分离C2H2。
Separation of acetylene (C2H2) from ethylene (C2H4) and carbon dioxide (CO2) is of great importance in the petrochemical industry but remains a daunting challenge due to their very similar sizes and physical properties. Although a number of porous materials have been developed as promising adsorbents for either C2H2/C2H4 or C2H2/CO2 separation, few materials exhibit simultaneously high selectivities for both gas mixtures. Herein, we report the use of a four-connected N-donor organic linker to construct a novel water-stable SIFSIX-type material, [Cu(TPB)SiF6](n) (termed ZJU-280, TPB = 1,2,4,5-tetra(pyridin-4-yl)benzene). This material features suitable rhombic pores and functional surfaces to interact optimally with C2H2 molecules, affording high C2H2 capture capacity and simultaneously high C2H2/CO2 (18.1) and C2H2/C2H4 (44.5) selectivities under ambient conditions. Theoretical calculations indicate that the suitable rhombic pores and functional sites can provide a multipoint binding environment to not only preferentially interact with C2H2 but also enable the dense packing of C2H2 molecules within the framework. Actual breakthrough experiments demonstrate that ZJU-280a can efficiently separate C2H2 from C2H2/CO2 (50/50, v/v) and C2H2/C2H4 (1/99 and 50/50) mixtures, respectively.