Covalent organic polymers based on special dithioureas for efficient removal of Hg2+ from aqueous solutions

IF 5.4 Q2 ENGINEERING, ENVIRONMENTAL
Haishan Zhu, Ye Tao, Cailing Ni, Yanqing Chen, Hualin Jiang, Yuancheng Qin
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Abstract

The damage caused by mercury ions (Hg2+) to human beings motivates the development of highly efficient technologies for the removal of Hg2+ from water. Here, based on the coordination theory between functional groups and Hg2+, two covalent organic polymers (COPs) materials were successfully prepared by a more environmentally friendly Michael addition elimination reaction, and the thiourea structure, which has a particularly strong affinity for Hg2+, was successfully introduced into the material framework. The introduction of the special dithiourea structure created a rich environment of S and N atoms within the COPs structure, which exhibited high adsorption performance for Hg2+. Adsorption experiments showed that the dithiourea-functionalized COPs exhibited high adsorption capacities for Hg2+, with the maximum adsorption capacities of 840.9 and 880 mg g−1 for the two materials, respectively. The adsorption performance remained relatively good after four adsorption-desorption cycles, and the adsorption selectivity for Hg2+ was intense. Mechanistic studies by X-ray photoelectron spectroscopy and density flooding theory calculations suggest that it is the S atoms within the structure that chelate with the Hg2+ and contribute to the adsorption capacity of the Hg2+. Therefore, this study provides a new strategy for the development of COP adsorbents for efficient removal of Hg2+ in aqueous solutions during remediation activities.

Abstract Image

基于特殊二硫代氨基脲的共价有机聚合物,用于从水溶液中高效去除 Hg2+
汞离子(Hg2+)对人类造成的伤害促使人们开发高效的技术来去除水中的 Hg2+。本文基于官能团与 Hg2+ 的配位理论,采用更环保的迈克尔加成消除反应成功制备了两种共价有机聚合物(COPs)材料,并成功地将对 Hg2+ 有特别强亲和力的硫脲结构引入到材料框架中。特殊二硫脲结构的引入在 COPs 结构中创造了丰富的 S 原子和 N 原子环境,对 Hg2+ 具有很高的吸附性能。吸附实验表明,二硫代尿素官能化 COPs 对 Hg2+ 具有很高的吸附容量,两种材料的最大吸附容量分别为 840.9 mg g-1 和 880 mg g-1。经过四次吸附-解吸循环后,吸附性能仍然较好,而且对 Hg2+ 的吸附选择性很强。通过 X 射线光电子能谱和密度泛滥理论计算进行的机理研究表明,是结构中的 S 原子与 Hg2+ 发生了螯合作用,从而提高了对 Hg2+ 的吸附能力。因此,这项研究为开发 COP 吸附剂提供了一种新策略,可在修复活动中有效去除水溶液中的 Hg2+。
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来源期刊
Journal of hazardous materials advances
Journal of hazardous materials advances Environmental Engineering
CiteScore
4.80
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