Liu Lizhen, Yao Zizhu, Ye Yingxiang, Yang Yike, Lin Quanjie, Zhang Zhangjing, O'Keeffe Michael, Xiang Shengchang
Fujian Provincial Key Laboratory of Polymer Materials, College of Chemistry and Materials Science, Fujian Normal University, 32 Shangsan Road, Fuzhou 350007, P. R. China.
College of Materials Science and Engineering, Key Laboratory of Polymer Materials and Products of Universities in Fujian, Fujian University of Technology, Fuzhou, Fujian 350118, P.R. China.
J Am Chem Soc. 2020 May 20;142(20):9258-9266. doi: 10.1021/jacs.0c00612. Epub 2020 May 7.
Introducing multiclusters and multiligands (mm) in a well-defined array will greatly increase the diversity of metal-organic frameworks (MOFs). Here, a series of porous mm-MOFs constructed from a pillared-layer and pore-space partition (PL-PSP) have been achieved. with {Co}-cluster-based sheets and {Co}-cluster-based pillars exhibits new (3,9,12)-connected topology. By using the substituted analogues of the ligands and metal ions, seven isoreticular mm-MOFs (, = PTB, TATB, Me-INA, F-INA, NDC, BrBDC, Ni) have been synthesized with the adjustable BET surface areas ranging from 731 to 1306 m/g as well as the adsorption capacity of CO increasing by 77%. The CH/CO mixture can be effectively separated in the breakthrough experiments in the fixed bed filled with solid at ambient temperature. In all, integrating pillared-layer strategy and pore-space partitioning is effective at constructing mm-MOFs with multivariate environments for the optimization of gas adsorption and separation.
在一个定义明确的阵列中引入多簇和多配体（mm）将极大地增加金属有机框架（MOF）的多样性。在此，已经实现了一系列由柱状层和孔空间分区（PL-PSP）构建的多孔mm-MOF。基于{Co}簇的片层和基于{Co}簇的柱体呈现出新的（3,9,12）连接拓扑结构。通过使用配体和金属离子的取代类似物，已经合成了七种等规mm-MOF（，=PTB、TATB、Me-INA、F-INA、NDC、BrBDC、Ni），其BET表面积可在731至1306 m²/g之间调节，并且CO的吸附容量增加了77%。在填充有固体的固定床中于环境温度下进行的突破实验中，CH₄/CO混合物能够被有效分离。总之，整合柱状层策略和孔空间分区对于构建具有多变量环境的mm-MOF以优化气体吸附和分离是有效的。
