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Construction of crystal defect sites in UiO-66 for adsorption of dimethyl phthalate and phthalic acid
Microporous and Mesoporous Materials ( IF 4.8 ) Pub Date : 2020-11-23 , DOI: 10.1016/j.micromeso.2020.110778
Peiming Wang , Liuxin Sun , Jiahua Ye , Qing Liu , Zhaoyang Fei , Xian Chen , Zhuxiu Zhang , Jihai Tang , Mifen Cui , Xu Qiao

The influence of constructed crystal defect sites in the metal-organic framework on the adsorptive removal of phthalic acid and dimethyl phthalate from aqueous solution has been investigated by etching UiO-66 with three monocarboxylic acids (MAs), including acetic acid (AA), trifluoroacetic acid (TFA) and trichloroacetic acid (TCA). The incomplete replacement of bridging ligands in UiO-66s by MAs, leading to the departure of partial ligands and metal clusters to create mesopores in metal organic frameworks, was determined by thermogravimetric analysis (TGA), nuclear magnetic resonance (1H NMR) and N2 adsorption-desorption. The results showed that mediate defect would increase the specific surface area and introduce mesopores to some extent, and the crystal structure was gradually destroyed as the excess concentration of MAs. Among UiO-66 samples, the UiO-66 etched by AA with concentration of 1.6 mol/L (UiO-66-1.6AA) had the highest specific surface area while the UiO-66-0.2TCA had the largest pore volume, which significantly enhanced the adsorption capacity for DMP and PA (18.05% up of PA and 41.59% up of DMP to UiO-66) respectively. The experimental data followed the pseudo-first-order kinetic and Langmuir model. In addition, regeneration study showed that the adsorption capacity of PA and DMP on UiO-66-0.2TCA and UiO-66-1.6AA can still remain over 83 and 90% after five cycles, respectively. The crystal defect sites introduction of mesopores by etching method would be an effective strategy to adsorptive removal of organic pollutants in aqueous solution.



中文翻译:

在UiO-66中构建晶体缺陷位点以吸附邻苯二甲酸二甲酯和邻苯二甲酸

通过用三种单羧酸(MA)(包括乙酸(AA),三氟乙酸)蚀刻UiO-66,研究了金属有机骨架中构造的晶体缺陷位点对从水溶液中吸附去除邻苯二甲酸和邻苯二甲酸二甲酯的影响。酸(TFA)和三氯乙酸(TCA)。通过热重分析(TGA),核磁共振(1 H NMR)和N确定了MAs在UiO-66s中桥接配体的不完全取代,导致部分配体和金属簇的离开,从而在金属有机骨架中形成中孔。2吸附-解吸。结果表明,中间缺陷会增加比表面积,并在一定程度上引入介孔,并且随着MAs浓度的增加,晶体结构逐渐被破坏。在UiO-66样品中,AA蚀刻浓度为1.6 mol / L的UiO-66(UiO-66-1.6AA)具有最高的比表面积,而UiO-66-0.2TCA具有最大的孔体积,增强了DMP和PA的吸附能力(PA分别对UiO-66的吸附量增加了18.05%,DMP的吸附量增加了41.59%)。实验数据遵循伪一阶动力学和Langmuir模型。此外,再生研究表明,PA和DMP在UiO-66-0.2TCA和UiO-66-1.6AA上的吸附能力在五个循环后仍分别保持在83%和90%以上。

更新日期:2020-11-23
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