Qin Lu-Zhu, Xiong Xiao-Hong, Wang Shi-Han, Zhang Liang, Meng Liu-Li, Yan Le, Fan Ya-Nan, Yan Tong-An, Liu Da-Huan, Wei Zhang-Wen, Su Cheng-Yong
MOE Laboratory of Bioinorganic and Synthetic Chemistry, Lehn Institute of Functional Materials, School of Chemistry, Sun Yat-Sen University, Guangzhou 510006, China.
State Key Laboratory of Organic-Inorganic Composites, Beijing University of Chemical Technology, Beijing 100029, China.
ACS Appl Mater Interfaces. 2022 Oct 12;14(40):45444-45450. doi: 10.1021/acsami.2c13446. Epub 2022 Sep 30.
Adsorptive separation based on porous solid adsorbents has emerged as an excellent effective alternative to energy-intensive conventional separation methods in a low energy cost and high working capacity manner. However, there are few stable mesoporous metal-organic frameworks (MOFs) for efficient purification of methane from other light hydrocarbons in natural gas. Herein, we report a series of stable mesoporous MOFs, MIL-101-Cr/Fe/Fe-NH, for efficient separation of CH and CH from a ternary mixture CH/CH/CH. Experimental results show that all three MOFs possess excellent thermal, acid/basic, and hydrothermal stability. Single-component adsorption suggested that they have high CH adsorption capacity and commendable selectivity for CH and CH over CH. Transient breakthrough experiments further certified the ability of direct separation of CH from simulated natural gas and indirect recovery of CH from the packing column. Theoretical calculations illustrated that the van der Waals force proportional to the molecular weight is the key factor and that the structural integrity and defect can impact separation performances.
基于多孔固体吸附剂的吸附分离已成为一种以低能耗和高工作容量的方式替代能源密集型传统分离方法的有效选择。然而,用于从天然气中的其他轻质烃类中高效纯化甲烷的稳定介孔金属有机框架(MOF)却很少。在此,我们报道了一系列稳定的介孔MOF,即MIL-101-Cr/Fe/Fe-NH,用于从三元混合物CH₄/C₂H₆/C₃H₈中高效分离CH₄和C₂H₆。实验结果表明,所有这三种MOF都具有出色的热稳定性、酸碱稳定性和水热稳定性。单组分吸附表明它们对CH₄具有高吸附容量,并且对C₂H₆和C₃H₈相对于CH₄具有良好的选择性。瞬态突破实验进一步证实了从模拟天然气中直接分离CH₄以及从填充柱中间接回收C₂H₆的能力。理论计算表明,与分子量成正比的范德华力是关键因素,并且结构完整性和缺陷会影响分离性能。