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具有转向介孔尺寸的分级孔 UiO-66-NH xerogel,用于高效去除有机污染物。

Hierarchical-pore UiO-66-NH xerogel with turned mesopore size for highly efficient organic pollutants removal.

机构信息

State Key Laboratory of Separation Membranes and Membrane Processes, Tiangong University, Tianjin 300387, China; School of Chemical Engineering and Technology, Tiangong University, Tianjin 300387, China.

State Key Laboratory of Separation Membranes and Membrane Processes, Tiangong University, Tianjin 300387, China; School of Chemical Engineering and Technology, Tiangong University, Tianjin 300387, China.

出版信息

J Colloid Interface Sci. 2022 Dec 15;628(Pt A):705-716. doi: 10.1016/j.jcis.2022.08.010. Epub 2022 Aug 3.

DOI:10.1016/j.jcis.2022.08.010
PMID:35944301
Abstract

Persistent organic pollutants in water are not only a potential threat to human health, but also cause damage to the ecological environment. Hence, the removal of large organic pollutants from wastewater is of great importance for environmental protection. Herein, hierarchical-pore UiO-66-NH xerogels (H-UiO-66-NH xerogels) with different mesopore size, H-UiO-66-NH-11.6 nm and H-UiO-66-NH-3.7 nm, were successfully synthesized by combining sol-gel-based method and acid modulator, featuring the characteristics of simple operation, rapid and scalable process, low cost, and the high space-time yield (STY). N adsorption-desorption isotherms reveal that the obtained H-UiO-66-NH xerogels possess high surface area, hierarchical-pore structures, large pore volume, and turntable mesopore size. Batch adsorption experiments demonstrate that H-UiO-66-NH-11.6 nm has excellent adsorption performance for reactive red 195 (RR 195) dye removal. The maximum adsorption capacity of H-UiO-66-NH-11.6 nm is 884.96 mg g, which is 4.7 times of the microporous UiO-66-NH (185.15 mg g). Moreover, the removal efficiency of H-UiO-66-NH-11.6 nm for RR 195 can exceed 99 %. The adsorption mechanism reveals that the excellent RR 195 capture stems from the large mesoporous structure and abundant adsorption sites provided by the Zr cluster and -NH groups in H-UiO-66-NH-11.6 nm. Besides, H-UiO-66-NH-11.6 nm also exhibits a much larger adsorption capacity for some other organic pollutants, such as tetracycline, reactive black 5, and amoxicillin, demonstrating that the H-UiO-66-NH xerogel has great potential for organic pollutant removal.

摘要

水中的持久性有机污染物不仅对人类健康构成潜在威胁,还会对生态环境造成破坏。因此,从废水中去除大有机污染物对于环境保护至关重要。在此,通过溶胶-凝胶法结合酸调节剂成功合成了具有不同介孔尺寸(H-UiO-66-NH-11.6nm 和 H-UiO-66-NH-3.7nm)的分级孔 UiO-66-NH 干凝胶(H-UiO-66-NH 干凝胶),其具有操作简单、快速、可扩展、成本低和时空产率(STY)高的特点。N2 吸附-脱附等温线表明,所得到的 H-UiO-66-NH 干凝胶具有高比表面积、分级孔结构、大孔体积和可旋转的介孔尺寸。批量吸附实验表明,H-UiO-66-NH-11.6nm 对活性红 195(RR195)染料的去除具有优异的吸附性能。H-UiO-66-NH-11.6nm 的最大吸附容量为 884.96mg·g-1,是微孔 UiO-66-NH(185.15mg·g-1)的 4.7 倍。此外,H-UiO-66-NH-11.6nm 对 RR195 的去除效率可超过 99%。吸附机理表明,Zr 簇和 H-UiO-66-NH-11.6nm 中的-NH 基团提供的大介孔结构和丰富的吸附位点是 RR195 出色捕获的原因。此外,H-UiO-66-NH-11.6nm 对其他一些有机污染物,如四环素、活性黑 5 和阿莫西林,也表现出更大的吸附容量,这表明 H-UiO-66-NH 干凝胶在去除有机污染物方面具有巨大的潜力。

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