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用于罗克沙砷水溶液快速可控脱除的金属有机骨架中的缺陷生成。

Defect creation in metal-organic frameworks for rapid and controllable decontamination of roxarsone from aqueous solution.

机构信息

Key Laboratory for Ultrafine Materials of Ministry of Education, School of Materials Science and Engineering, East China University of Science and Technology, Shanghai 200237, China.

Murad Research Center for Modernized Chinese Medicine, Shanghai University of Traditional Chinese Medicine, Shanghai 201203, China.

出版信息

J Hazard Mater. 2016 Jan 25;302:57-64. doi: 10.1016/j.jhazmat.2015.09.040. Epub 2015 Sep 25.

DOI:10.1016/j.jhazmat.2015.09.040
PMID:26444487
Abstract

Given the great harm to the human health of organic arsenic compounds (OACs), developing highly efficient adsorbents with both rapid adsorption rate and high saturation capacity is paramount important. Herein, Zr-based metal-organic frameworks (MOFs) of UiO-66 have been successfully exploited for the efficient decontamination of a typical organic arsenic compound of roxarsone (ROX) from aqueous solution. The influences of the most significant parameters such as contact time, adsorbate concentration, pH as well as ionic strength on the adsorption of ROX were investigated. The amount of missing-linker defects in UiO-66 was systematically tuned by changing the concentration of modulator in the reactants. The presence of the defects not only resulted in the dramatically enhanced porosity, but also induced the creation of ZrOH groups which served as the main active adsorption sites for efficient ROX sequestration. As a result, adsorptive capacity of ROX over UiO-66 could be improved to 730 mg/g, which was much higher than those of many reported adsorbents. Meanwhile, the adsorption equilibrium time could be reduced to as short as 30 min. These merits, combined with their excellent stability, prefigure the great potentials of these defect-tunable UiO-66 MOFs as adsorbents for the efficient removal of various OACs from the polluted water.

摘要

鉴于有机砷化合物(OACs)对人类健康的巨大危害,开发具有快速吸附速率和高饱和容量的高效吸附剂至关重要。在此,我们成功地利用基于锆的金属有机骨架(MOFs)UiO-66 从水溶液中有效去除典型的有机砷化合物罗硝唑(ROX)。研究了接触时间、吸附剂浓度、pH 值和离子强度等最显著参数对 ROX 吸附的影响。通过改变反应物中调节剂的浓度,系统地调节了 UiO-66 中缺失连接体的缺陷数量。缺陷的存在不仅导致了孔隙率的显著增强,而且还诱导了 ZrOH 基团的形成,这些基团是有效 ROX 螯合的主要活性吸附位点。结果,ROX 在 UiO-66 上的吸附容量可提高到 730mg/g,远高于许多已报道的吸附剂。同时,吸附平衡时间可缩短至 30min 以内。这些优点,再加上其优异的稳定性,预示着这些可调节缺陷的 UiO-66 MOFs 作为吸附剂,具有从受污染的水中高效去除各种 OACs 的巨大潜力。

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