Fan Weidong, Yuan Shuai, Wang Wenjing, Feng Liang, Liu Xiuping, Zhang Xiurong, Wang Xia, Kang Zixi, Dai Fangna, Yuan Daqiang, Sun Daofeng, Zhou Hong-Cai
School of Materials Science and Engineering, College of Science, China University of Petroleum (East China), Qingdao, Shandong 266580, China.
Department of Chemistry, Materials Science and Engineering, Texas A&M University, College Station, Texas 77842-3012, United States.
J Am Chem Soc. 2020 May 13;142(19):8728-8737. doi: 10.1021/jacs.0c00805. Epub 2020 Mar 27.
Adsorptive separation of acetylene (CH) from carbon dioxide (CO) promises a practical way to produce high-purity CH required for industrial applications. However, challenges exist in the pore environment engineering of porous materials to recognize two molecules due to their similar molecular sizes and physical properties. Herein, we report a strategy to optimize pore environments of multivariate metal-organic frameworks (MOFs) for efficient CH/CO separation by tuning metal components, functionalized linkers, and terminal ligands. The optimized material UPC-200(Al)-F-BIM, constructed from Al clusters, fluorine-functionalized organic linkers, and benzimidazole terminal ligands, demonstrated the highest separation efficiency (CH/CO uptake ratio of 2.6) and highest CH productivity among UPC-200 systems. Experimental and computational studies revealed the contribution of small pore size and polar functional groups on the CH/CO selectivity and indicated the practical CH/CO separation of UPC-200(Al)-F-BIM.
从二氧化碳（CO₂）中吸附分离乙炔（C₂H₂）有望成为一种生产工业应用所需高纯度C₂H₂的实用方法。然而，由于多孔材料中两种分子的尺寸和物理性质相似，在其孔环境工程中识别这两种分子存在挑战。在此，我们报告了一种通过调整金属成分、功能化连接体和末端配体来优化多元金属有机框架（MOF）孔环境以实现高效C₂H₂/CO₂分离的策略。由铝簇、氟功能化有机连接体和苯并咪唑末端配体构建的优化材料UPC-200(Al)-F-BIM在UPC-200体系中展现出最高的分离效率（C₂H₂/CO₂吸附比为2.6）和最高的C₂H₂生产率。实验和计算研究揭示了小孔径和极性官能团对C₂H₂/CO₂选择性的贡献，并表明UPC-200(Al)-F-BIM在实际C₂H₂/CO₂分离中的应用。
