Combination of Low-Polar and Polar Binding Sites in Aliphatic MOFs for the Efficient C2H6/C2H4 Separation.
Combination of Low-Polar and Polar Binding Sites in Aliphatic MOFs for the Efficient C2H6/C2H4 Separation.
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DOI：
10.1021/acsami.2c21261
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发表时间：
2023-01
影响因子：
9.5
通讯作者：
Jingyi Zhou;Tian Ke;Xiaoqian Zhu;Binhao Jin;Zongbi Bao;Zhiguo Zhang;Yiwen Yang;Qilong Ren;Qiwei Yang
中科院分区：
文献类型：
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作者：
Jingyi Zhou;Tian Ke;Xiaoqian Zhu;Binhao Jin;Zongbi Bao;Zhiguo Zhang;Yiwen Yang;Qilong Ren;Qiwei Yang
从C2 H6/C2 H4混合物中选择性捕获C2 H6对于实现C2 H4的有效一步纯化至关重要，但由于它们相似的性质和较小的C2 H6四极矩通常导致C2 H4优先吸附，因此仍然具有挑战性。本文中，我们报道了两个同构柱撑层金属有机骨架，ZUL-C3和ZUL-C4，它们是由混合多环烷烃型配体构建的。它们的低极性孔环境沿着孔表面更易接近的低极性C-H结合位点，有利于与C2 H6产生更多的货车范德华相互作用，而分布在孔四角的羧基与C2 H6形成更强、更偶极的相互作用，在静态吸附实验中，ZUL-C3和ZUL-C4的C2 H6/C2 H4吸收比分别为1.50和1.72，突破性实验中，等摩尔C2 H6/C2 H4混合物的ZUL-C3生产率为10.1 L/kg，ZUL-C4生产率为14.6 L/kg（纯度>99.99%）。
The selective capture of C2H6 from C2H6/C2H4 mixtures is of critical importance to realize the efficient one-step purification of C2H4 but remains challenging due to their similar properties and smaller quadrupole moment of C2H6 that usually result in C2H4-preferring adsorption. Herein, we reported two isostructural pillared-layer metal-organic frameworks, ZUL-C3 and ZUL-C4, which were constructed by mixed polycycloalkane-type ligands. Their low-polar pore environment along with more accessible low-polar C-H binding sites on the pore surface are conducive to generate more van der Waals interactions with C2H6 while the carboxylic groups distributed at four corners of pores form stronger and more dipolar interactions with C2H6, cooperatively resulting in a good C2H6/C2H4 uptake ratio of 1.50 for ZUL-C3 and 1.72 for ZUL-C4 in static adsorption experiments and a high C2H4 (>99.99% purity) productivity of 10.1 L/kg for ZUL-C3 and 14.6 L/kg for ZUL-C4 from an equimolar C2H6/C2H4 mixture in breakthrough experiments.