Wang Gang-Ding, Li Yong-Zhi, Krishna Rajamani, Zhang Wen-Yan, Hou Lei, Wang Yao-Yu, Zhu Zhonghua
Key Laboratory of Synthetic and Natural Functional Molecule of the Ministry of Education, College of Chemistry & Materials Science, Northwest University, Xi'an, 710069, P. R. China.
School of Materials and Physics, China University of Mining and Technology, Xuzhou, 221116, P. R. China.
Angew Chem Int Ed Engl. 2024 Apr 8;63(15):e202319978. doi: 10.1002/anie.202319978. Epub 2024 Mar 1.
Ethylene (CH) purification and propylene (CH) recovery are highly relevant in polymer synthesis, yet developing physisorbents for these industrial separation faces the challenges of merging easy scalability, economic feasibility, high moisture stability with great separation efficiency. Herein, we reported a robust and scalable MOF (MAC-4) for simultaneous recovery of CH and CH. Through creating nonpolar pores decorated by accessible N/O sites, MAC-4 displays top-tier uptakes and selectivities for CH and CH over CH at ambient conditions. Molecular modelling combined with infrared spectroscopy revealed that CH and CH molecules were trapped in the framework with stronger contacts relative to CH. Breakthrough experiments demonstrated exceptional separation performance for binary CH/CH and CH/CH as well as ternary CH/CH/CH mixtures, simultaneously affording record productivities of 27.4 and 36.2 L kg for high-purity CH (≥99.9 %) and CH (≥99.5 %). MAC-4 was facilely prepared at deckgram-scale under reflux condition within 3 hours, making it as a smart MOF to address challenging gas separations.
乙烯（CH）纯化和丙烯（CH）回收在聚合物合成中具有高度相关性，然而，开发用于这些工业分离的物理吸附剂面临着将易于扩展、经济可行性、高湿度稳定性与高分离效率相结合的挑战。在此，我们报道了一种用于同时回收CH和CH的坚固且可扩展的金属有机框架材料（MOF，MAC-4）。通过创建由可及的N/O位点修饰的非极性孔，MAC-4在环境条件下对CH和CH相对于CH显示出顶级的吸附量和选择性。分子模拟结合红外光谱表明，CH和CH分子相对于CH以更强的相互作用被困在框架中。突破实验证明了其对二元CH/CH和CH/CH以及三元CH/CH/CH混合物具有出色的分离性能，同时为高纯度CH（≥99.9%）和CH（≥99.5%）提供了创纪录的生产率，分别为27.4和36.2 L kg。MAC-4在回流条件下3小时内即可轻松地以克级规模制备，使其成为解决具有挑战性的气体分离问题的智能MOF。
