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简便合成巯基改性共价有机框架材料用于高效去除水中 Hg(II)。

Facile synthesis of sulfhydryl modified covalent organic frameworks for high efficient Hg(II) removal from water.

机构信息

The Key Laboratory of Water and Sediment Sciences, Ministry of Education, College of Environmental Sciences and Engineering, Peking University, Beijing 100871, PR China.

The Key Laboratory of Water and Sediment Sciences, Ministry of Education, College of Environmental Sciences and Engineering, Peking University, Beijing 100871, PR China.

出版信息

J Hazard Mater. 2021 Mar 5;405:124190. doi: 10.1016/j.jhazmat.2020.124190. Epub 2020 Oct 6.

Abstract

In present study, we fabricated sulfhydryl modified covalent organic frameworks (COF-‒SH) through one-step reaction for the removal of Hg(II) from water. Different techniques were employed to characterize the fabricated COFs. We find that COF-‒SH exhibits great adsorption capacity (1283 mg/g) towards Hg(II), which is over 25 times higher than that of COF-1 without ‒-SH (53.1 mg/g). COF-SH has fast adsorption kinetics with the removal of 95% of 1000 μg/L Hg(II) within 30 min and over 99% after 2 h. Under a wide pH range (from 4 to 9), COF-‒SH exhibits high removal efficiencies (>99%). Moreover, COF-SH can selectively adsorb Hg(II) in the presence of other metal cations up to 1000 μg/L. X-ray photoelectron spectroscopy analysis reveals the presence of high affinity between thiol-S atom and Hg(II), which is also responsible for the high selectivity towards Hg(II) compared with other cations. Because of the transfer from enol form to keto form during synthesis, COF-SH exhibit remarkable stability during 10-cycle regeneration and reuse test. During utilization in wastewater extracted from Hg contaminated sludge, COF-‒SH displays high Hg(II) removal efficiency (>95%) under multiple coexisting ions conditions. The results suggest that COF-‒SH have great potential for Hg(II) removal from water under complex conditions.

摘要

在本研究中,我们通过一步反应制备了巯基改性的共价有机框架(COF-SH),用于从水中去除 Hg(II)。采用了不同的技术对制备的 COFs 进行了表征。我们发现 COF-SH 对 Hg(II)具有很强的吸附能力(1283 mg/g),是没有‒-SH 的 COF-1 的 25 倍以上(53.1 mg/g)。COF-SH 具有快速的吸附动力学,在 30 min 内可去除 1000μg/L Hg(II)的 95%,2 h 后可去除 99%以上。在很宽的 pH 范围(4 至 9)内,COF-SH 的去除效率都很高(>99%)。此外,COF-SH 可以在存在其他金属阳离子(高达 1000μg/L)的情况下选择性地吸附 Hg(II)。X 射线光电子能谱分析表明,巯基-S 原子与 Hg(II)之间存在高亲和力,这也是与其他阳离子相比对 Hg(II)具有高选择性的原因。由于在合成过程中从烯醇形式转变为酮式,COF-SH 在 10 次循环再生和重复使用测试中表现出显著的稳定性。在从 Hg 污染污泥中提取的废水中进行利用时,COF-SH 在多种共存离子条件下仍可保持很高的 Hg(II)去除效率(>95%)。结果表明,COF-SH 在复杂条件下具有从水中去除 Hg(II)的巨大潜力。

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