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用于从单/二元溶液中高效共固定砷酸盐和氟化物的缺陷型 UiO-66 的合成与表征。

Synthesis and characterization of defective UiO-66 for efficient co-immobilization of arsenate and fluoride from single/binary solutions.

机构信息

Department of Earth Resources Engineering, Faculty of Engineering, Kyushu University, Fukuoka, 819-0395, Japan; Department of Earth Resources and Environmental Engineering, Hanyang University, 222 Wangsimni-ro, Seongdong-gu, Seoul, 04763, South Korea.

Department of Earth Resources Engineering, Faculty of Engineering, Kyushu University, Fukuoka, 819-0395, Japan.

出版信息

Environ Pollut. 2021 Jun 1;278:116841. doi: 10.1016/j.envpol.2021.116841. Epub 2021 Mar 1.

Abstract

Here, we aimed to synthesize UiO-66 architected fumaric acid mediated lanthanum (La-fum), zirconium (Zr-fum), and cerium (Ce-fum) metal-organic frameworks (MOFs) for co-immobilizations of both arsenate and fluoride from both single and binary systems. The crystalline behavior of Zr-fum MOF was the lowest compared to the other two forms, due to the fact that it required a modulator support as the nucleus growth nature of zirconium moiety is different. The Langmuir maximum adsorption densities of arsenate (fluoride) were 2.689 (4.240), 1.666 (2.255), and 2.174 (4.155) mmol/g for La-fum, Zr-fum, and Ce-fum, respectively and these adsorption densities were found to have record-high values compared with the existing materials in the literature. The arsenate and fluoride adsorption on the MOF materials were confirmed by XPS, PXRD and FTIR studies. The arsenate adsorption mechanism on La-fum and Ce-fum through monodentate complexation confirmed using the distinguished K-edge shell distance in EXAFS studies. The arsenate and fluoride-sorbed materials were recycled using 0.01 M HNO and were further utilized for six consecutive cycles for both arsenate and fluoride adsorption indicated the feasibility of the materials. This kind of facile and easy solvothermal synthesized MOFs could pave a way towards the removal of toxins in a practical wastewater as these have superior adsorption properties, stability and reusability.

摘要

在这里,我们旨在合成 UiO-66 结构的富马酸介导的镧(La-fum)、锆(Zr-fum)和铈(Ce-fum)金属-有机骨架(MOFs),以从单一组分和二元体系中共同固定砷酸盐和氟化物。与其他两种形式相比,Zr-fum MOF 的结晶行为最低,这是因为它需要调节剂支持,因为锆部分的核生长性质不同。La-fum、Zr-fum 和 Ce-fum 对砷酸盐(氟化物)的朗缪尔最大吸附密度分别为 2.689(4.240)、1.666(2.255)和 2.174(4.155)mmol/g,这些吸附密度与文献中现有的材料相比具有创纪录的高值。通过 XPS、PXRD 和 FTIR 研究证实了 MOF 材料对砷酸盐和氟化物的吸附。通过 EXAFS 研究中独特的 K 边壳距离证实了 La-fum 和 Ce-fum 通过单齿络合对砷酸盐的吸附机理。使用 0.01 M HNO 回收吸附了砷酸盐和氟化物的材料,并进一步将其用于砷酸盐和氟化物吸附的六个连续循环,表明了材料的可行性。这种简便且易于溶剂热合成的 MOFs 可以为实际废水中的毒素去除铺平道路,因为它们具有优越的吸附性能、稳定性和可重复使用性。

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