Fabrication of (4,10) and (4,12)-Connected Multifunctional Zirconium Metal-Organic Frameworks for the Targeted Adsorption of a Guest Molecule

Fabrication of (4,10) and (4,12)-Connected Multifunctional Zirconium Metal-Organic Frameworks for the Targeted Adsorption of a Guest Molecule
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用于客体分子靶向吸附的 (4,10) 和 (4,12) 连接多功能锆金属有机框架的制备

DOI:
10.1021/acs.inorgchem.9b02950
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发表时间:
2020
影响因子:
4.6
通讯作者:
Huang Wei
Huang Wei
中科院分区:
化学2区
文献类型:
--
作者:
Zhang Liangliang;Guo Bingbing;He Huihui;Zhang Xiurong;Feng Yang;Fan Weidong;Cao Junlong;Lu Guang;Chen Yanhui;Sun Daofeng;Huang Wei

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根据拓扑导向的原理,合成了一种以四甲基(4,4 ′,4 ″,4 ′-(吡嗪-2,3,5,6-四基))四苯甲酸(H4 TPTA)为配体、以8-连接的Zr 6(μ3-OH)8(OH)8]8+为簇合物的具有C2对称性的锆多功能荧光体(PCN-207). PCN-206也可以通过调节苯甲酸的使用以改变H4 TPTA配体的柔性来获得。8-连接的Zr 6簇在流体和流体网络中的独特位置和四位初级连接体的灵活性使得能够在一锅反应中精确插入富马酸(FA)、1,4-苯二甲酸(H2 BDC)甚至2,6-萘二甲酸(H2 NDC)。辅助连接体用于产生新的MOF结构或拓扑结构或分裂孔隙空间,这可以显著改变支架MOF的孔隙率以及化学和物理性质。研究结果为多组分Zr-MOFs的合理设计提供了一种成功的策略。由于结构之间组成和构型的差异,PCN-207表现出最高的轻烃分离能力; PCN-206表现出目前MOFs中最高的2,4-D和DCF吸附能力。
Following the principle of a topology guide, a zirconium MOF (PCN-207) based on the H4TPTA ligand (tetramethyl(4,4′,4″,4‴-(pyrazine-2,3,5,6-tetrayl))tetrabenzoic acid) withC2symmetry and an 8-connected Zr6(μ3-OH)8(OH)8]8+cluster withD4hsymmetry has been synthesized. PCN-206 can also be obtained by modulating the benzoic acid usage to change the flexibility of the H4TPTA ligand. The unique positions of 8-connected Zr6clusters in thefluandscunetworks and the flexibility of the tetratopic primary linker enable the precise insertion of fumarate (FA), 1,4-benzenedicarboxylic acid (H2BDC), and even 2,6-naphthalenedicarboxylic acid (H2NDC) in a one-pot reaction. Auxiliary linkers are used to generate new MOF structures or topologies or to split the pore spaces, which may significantly change the porosity and chemical and physical properties of scaffold MOFs. The results provide a successful strategy for the rational design of multicomponent Zr-MOFs. Because of differences in composition and configuration between structures, PCN-207 shows the highest separation capability of light hydrocarbons; moreover, PCN-206 exhibits the highest adsorption capacity of 2,4-D and DCF among MOFs at present.