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基于新型三嗪的阳离子型共价有机聚合物用于高效选择性去除受污染水中的硒酸盐。

Novel triazine-based cationic covalent organic polymers for highly efficient and selective removal of selenate from contaminated water.

机构信息

Key Laboratory of Radiation Physics and Technology of the Ministry of Education, Institute of Nuclear Science and Technology, College of Chemistry, Sichuan University, Chengdu 610064, China.

Key Laboratory of Radiation Physics and Technology of the Ministry of Education, Institute of Nuclear Science and Technology, College of Chemistry, Sichuan University, Chengdu 610064, China.

出版信息

J Hazard Mater. 2022 Aug 15;436:129127. doi: 10.1016/j.jhazmat.2022.129127. Epub 2022 May 12.

Abstract

Selenium (Se) removal from contaminated water has become a major environmental problem in recent years. Designing efficient and selective materials for selenium adsorption is urgent and still represents a great challenge. Herein, two novel cationic covalent triazine frameworks (CTFS-Cl and CTFL-Cl) are developed for the first time and employed as a new class of Se adsorbents. The results from systematic adsorption experiments indicate that these materials can adsorb SeO in a wide range of pH values (2-11) with fast kinetics (5 min), outstanding adsorption capacity, and excellent selectivity over other competing anions. The maximum adsorption capacity achieved (149.3 mg/g by CTFS-Cl) constitutes one of the highest values among the organic polymeric materials. More importantly, after a single step adsorption, these materials can reduce the Se concentrations to lower than 10 μg/L, the lowest drinking water standard in the world. The adsorption mechanism was probed by XPS technique, EDS analysis, adsorption experiments, and DFT calculations, which reveals that anion exchange between Cl and SeO is the main driving force for Se adsorption. Additionally, CTFS-Cl and CTFL-Cl perform well toward real contaminated river water sample with the residual Se being less than 8.49 μg/L. This work demonstrates the excellent performance of CTFs-based materials with great application prospect for Se removal in contaminated water treatment.

摘要

近年来,从受污染的水中去除硒已成为一个主要的环境问题。设计高效和选择性的材料来吸附硒是紧迫的,仍然是一个巨大的挑战。在此,首次开发了两种新型的阳离子共价三嗪框架(CTFS-Cl 和 CTFL-Cl),并将其用作一类新型的硒吸附剂。系统的吸附实验结果表明,这些材料可以在很宽的 pH 值范围内(2-11)以快速动力学(5 分钟)吸附 SeO,具有出色的吸附容量和对其他竞争阴离子的优异选择性。通过 CTFS-Cl 实现的最大吸附容量(149.3mg/g)是有机聚合物材料中最高值之一。更重要的是,经过单次吸附,这些材料可以将硒浓度降低到低于 10μg/L,这是世界上最低的饮用水标准。通过 XPS 技术、EDS 分析、吸附实验和 DFT 计算探测吸附机制,揭示了 Cl 和 SeO 之间的阴离子交换是吸附硒的主要驱动力。此外,CTFS-Cl 和 CTFL-Cl 在实际受污染河水样本中表现良好,残留硒含量低于 8.49μg/L。这项工作展示了基于 CTFs 的材料的优异性能,在受污染水处理中去除硒具有广阔的应用前景。

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