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An NH2-modified {EuIII2}–organic framework for the efficient chemical fixation of CO2 and highly selective sensing of 2,4,6-trinitrophenol
Inorganic Chemistry Frontiers ( IF 7 ) Pub Date : 2021-08-04 , DOI: 10.1039/d1qi00762a
Hongtai Chen 1 , Zhengguo Zhang 1 , Tuoping Hu 1 , Xiutang Zhang 1
Affiliation  

In most instances, the incursion of functional groups on the inner surface of microporous MOFs could undoubtedly result in a significant improvement of their desirable performances, inspired by which one amino-functionalized ligand 2,6-di(3,5-dicarboxylphenyl)-4-aminobenzoic acid (H5DDAC) was designed and synthesized. By employing H5DDAC as the organic linker, the exquisite combination of dinuclear [Eu2(CO2)9] and [Eu2(CO2)6(H2O)2] generated one highly robust microporous framework of {(Me2NH2)4[Eu4(DDAC)3(HCO2)(OH2)2]·8DMF·9H2O}n (NUC-41), which was characterized by hierarchical channels and cage-like voids. Owing to the Lewis acid-base synergistic effect including open metal sites, free oxygen atoms and amino groups, NUC-41 with the aid of cocatalyst n-Bu4NBr exhibited extremely high catalytic activity for the cycloaddition reactions of alkyl epoxides and CO2 under mild solvent-free conditions, especially for epoxides with a smaller size. Furthermore, fluorescence experiments confirmed that the amino-functionalized skeleton of NUC-41 could effectively sense 2,4,6-trinitrophenol in aqueous solution over other nitro analytes including TNP, 2,4-DNP, 4-NP, 2,4-DNT, TNT, 1,4-DNB, 4-NT and NB with KSV and the limit of detection being 8.6 × 104 M−1 and 3.5 × 10−6 M, respectively. Therefore, these results indicate that amino functionalization is an effective strategy to improve and expand the application performance of MOFs, which is critically related to the sustainable development of MOF research in this day and age.

中文翻译:

NH2 修饰的 {EuIII2}-有机框架,用于有效化学固定 CO2 和高选择性传感 2,4,6-三硝基苯酚

在大多数情况下,微孔 MOF 内表面官能团的侵入无疑会显着提高其理想性能,其中一种氨基官能化配体 2,6-二(3,5-二羧基苯基)-4 -氨基苯甲酸(H 5 DDAC)被设计和合成。通过采用 H 5 DDAC 作为有机连接体,双核 [Eu 2 (CO 2 ) 9 ] 和 [Eu 2 (CO 2 ) 6 (H 2 O) 2 ]的巧妙结合产生了一种高度坚固的 {(Me 2 NH 2 ) 4 [Eu4 (DDAC) 3 (HCO 2 )(OH 2 ) 2 ]·8DMF·9H 2 O} n ( NUC-41 ),其特征在于分级通道和笼状空隙。由于路易斯酸-碱的协同效应,包括开放的金属位点,游离氧原子和氨基, NUC-41与助催化剂的辅助下Ñ -Bu 4 NBR表现出非常高的催化活性为烷基环氧化物的环加成反应和CO 2下温和的无溶剂条件,特别是对于较小尺寸的环氧化物。此外,荧光实验证实了氨基功能化的骨架与其他硝基分析物(包括 TNP、2,4-DNP、4-NP、2,4-DNT、TNT、1,4-DNB、4-NT)相比,NUC-41可以有效地检测水溶液中的 2,4,6-三硝基苯酚和NB,K SV和检测限分别为8.6 × 10 4 M -1和3.5 × 10 -6 M。因此,这些结果表明氨基功能化是提高和扩展 MOF 应用性能的有效策略,这与当今 MOF 研究的可持续发展密切相关。
更新日期:2021-08-19
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