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A Robust Hydrogen-Bonded Metal–Organic Framework with Enhanced Ethane Uptake and Selectivity
Chemistry of Materials ( IF 7.2 ) Pub Date : 2021-07-19 , DOI: 10.1021/acs.chemmater.1c01892 Minjung Kang 1 , Dong Won Kang 1 , Jong Hyeak Choe 1 , Hyojin Kim 1 , Dae Won Kim 1 , Hyein Park 1 , Chang Seop Hong 1
Chemistry of Materials ( IF 7.2 ) Pub Date : 2021-07-19 , DOI: 10.1021/acs.chemmater.1c01892 Minjung Kang 1 , Dong Won Kang 1 , Jong Hyeak Choe 1 , Hyojin Kim 1 , Dae Won Kim 1 , Hyein Park 1 , Chang Seop Hong 1
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Selective adsorption of trace C2H6 over C2H4 is important for the industrial purification of polymer-grade C2H4 (>99.95% purity). For practical applications, potential adsorbents show high structural stability while maintaining elevated C2H6 adsorption even at low pressures. Herein, we report a C2H6-selective metal–organic framework (MOF), viz., Co(AIN)2 (HAIN = 3-aminoisonicotinic acid), with a twofold interpenetrated dia structure. Compared to an isoreticular and unstable Co(IN)2 (HIN = isonicotinic acid) without internal hydrogen bonding, this framework exhibits exceptional structural robustness even under humid conditions because of the presence of intra- and inter-net hydrogen bonds between carboxylate oxygens and amino groups of AIN–. Decoration of the internal polar pore surfaces with groups that form extensive hydrogen bonds offers a more favorable environment for selective C2H6 adsorption. According to the ideal adsorbed solution theory, the predicted selectivity for C2H6/C2H4 was found to be 2.98 in C2H6/C2H4 (1:15, v/v) mixtures, which surpasses even the best-performing MOFs. The C2H6 uptake at 62.5 mbar partial pressure in the single-component isotherm, in C2H6/C2H4 (1:15, v/v) mixtures, was the highest (63.16 cm3 g–1) among MOF adsorbents, along with a nearly top-tier separation potential (116.03 cm3 g–1). Molecular modeling illustrates that the C–H···π interactions of C2H6 with the pore walls are more significant than those of C2H4, accounting for the improved selectivity for C2H6 over C2H4 in Co(AIN)2. The separation performance under dynamic dry and humid conditions was confirmed by breakthrough experiments. Co(AIN)2 was shown to be synthesized on a gram scale and was easily regenerated by inert gas purging. Thus, we demonstrated that coating of internal pore surfaces with groups that form hydrogen bonds provides more favorable environments for enhanced structural stability and C2H6 affinity and selectivity.
中文翻译：
具有增强的乙烷吸收和选择性的坚固的氢键金属-有机框架
在 C 2 H 4 上选择性吸附痕量 C 2 H 6对于聚合物级 C 2 H 4（>99.95% 纯度）的工业纯化很重要。对于实际应用，潜在的吸附剂显示出高结构稳定性，同时即使在低压下也能保持较高的 C 2 H 6吸附。在此，我们报告了一种 C 2 H 6 -选择性金属有机骨架 (MOF)，即Co(AIN) 2 (HAIN = 3-氨基异烟酸)，具有双重互穿dia结构。与等网状且不稳定的Co(IN) 2 相比（HIN =异烟酸）无内部氢键，该框架呈现即使在由于羧酸酯氧与AIN的氨基之间内和网间氢键的存在的潮湿的条件下特殊的结构坚固性- 。用形成大量氢键的基团装饰内部极性孔表面为选择性C 2 H 6吸附提供了更有利的环境。根据理想吸附溶液理论，C 2 H 6 /C 2 H 4中 C 2 H 6 /C 2 H 4的预测选择性为2.98(1:15, v/v) 混合物，甚至超过了性能最好的 MOF。在 C 2 H 6 /C 2 H 4 (1:15, v/v) 混合物中，单组分等温线在 62.5 mbar 分压下的 C 2 H 6吸收量最高 (63.16 cm 3 g –1 )在 MOF 吸附剂中，以及接近顶级的分离潜力 (116.03 cm 3 g –1 )。分子模型表明，C 2 H 6与孔壁的 C–H···π 相互作用比 C 2 H 4 的相互作用更显着，从而提高了对 C 的选择性2 ħ 6对C 2 H ^ 4中的Co（AIN）2。突破性实验证实了动态干湿条件下的分离性能。Co(AlN) 2显示为克级合成，并且很容易通过惰性气体吹扫再生。因此，我们证明了用形成氢键的基团涂覆内部孔表面为增强的结构稳定性和C 2 H 6亲和力和选择性提供了更有利的环境。
更新日期：2021-08-10
中文翻译：
具有增强的乙烷吸收和选择性的坚固的氢键金属-有机框架
在 C 2 H 4 上选择性吸附痕量 C 2 H 6对于聚合物级 C 2 H 4（>99.95% 纯度）的工业纯化很重要。对于实际应用，潜在的吸附剂显示出高结构稳定性，同时即使在低压下也能保持较高的 C 2 H 6吸附。在此，我们报告了一种 C 2 H 6 -选择性金属有机骨架 (MOF)，即Co(AIN) 2 (HAIN = 3-氨基异烟酸)，具有双重互穿dia结构。与等网状且不稳定的Co(IN) 2 相比（HIN =异烟酸）无内部氢键，该框架呈现即使在由于羧酸酯氧与AIN的氨基之间内和网间氢键的存在的潮湿的条件下特殊的结构坚固性- 。用形成大量氢键的基团装饰内部极性孔表面为选择性C 2 H 6吸附提供了更有利的环境。根据理想吸附溶液理论，C 2 H 6 /C 2 H 4中 C 2 H 6 /C 2 H 4的预测选择性为2.98(1:15, v/v) 混合物，甚至超过了性能最好的 MOF。在 C 2 H 6 /C 2 H 4 (1:15, v/v) 混合物中，单组分等温线在 62.5 mbar 分压下的 C 2 H 6吸收量最高 (63.16 cm 3 g –1 )在 MOF 吸附剂中，以及接近顶级的分离潜力 (116.03 cm 3 g –1 )。分子模型表明，C 2 H 6与孔壁的 C–H···π 相互作用比 C 2 H 4 的相互作用更显着，从而提高了对 C 的选择性2 ħ 6对C 2 H ^ 4中的Co（AIN）2。突破性实验证实了动态干湿条件下的分离性能。Co(AlN) 2显示为克级合成，并且很容易通过惰性气体吹扫再生。因此，我们证明了用形成氢键的基团涂覆内部孔表面为增强的结构稳定性和C 2 H 6亲和力和选择性提供了更有利的环境。
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