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巯基/甲基硫基功能化多孔芳香骨架用于同时从水中捕获芳香族污染物和 Hg(II)。

Thiol/methylthio-functionalized porous aromatic frameworks for simultaneous capture of aromatic pollutants and Hg(II) from water.

机构信息

College of Chemistry and Chemical Engineering, Hubei Key Laboratory of Biomass Fibers and Eco-dyeing and Finishing, Wuhan Textile University, Wuhan 430073, China.

College of Chemistry and Chemical Engineering, Hubei Key Laboratory of Biomass Fibers and Eco-dyeing and Finishing, Wuhan Textile University, Wuhan 430073, China.

出版信息

J Hazard Mater. 2021 Sep 15;418:126244. doi: 10.1016/j.jhazmat.2021.126244. Epub 2021 Jun 1.

Abstract

Simultaneously capturing organic pollutants and heavy metal can greatly reduce the water remediation time and cost, however it is still a great challenge presently. Herein, two novel thiol/methylthio-functionalized porous aromatic frameworks were synthesized as sorbents via the Sonogashira-Hagihara reaction of 1,3,5-triethynylbenzene and 1,3,5-tris(4-bromophenyl) benzene, the subsequent chloromethylation of the phenyl rings, and the final nucleophile substitution of -Cl groups by NaSH/NaSMe. These two sorbents were characterized by FT-IR spectra, energy dispersive X-ray spectra, scanning electron microscope, nitrogen adsorption analysis, thermo-gravimetric analysis, and elemental analyses. Adsorption experiments displayed that new sorbents had high uptake abilities and fast adsorption kinetics for aromatic pollutants and mercury (II) (Hg(II)). The maximum adsorption capacity (Q) of toluene and m-xylene on both new sorbents were 531.9-571.4 mg/g with the kinetic binding rate constants (k) of 0.00276-0.02422 g/mg/min, and the Q values of Hg(II) were 148.1-180.3 mg/g with k of 0.00592-0.01573 g/mg/min. Moreover, new sorbents indicated high simultaneous uptake abilities for these pollutants with good reusability, and finally they were successfully applied to the simultaneous remediation of these pollutants in two simulated sewages with high and low concentration, indicating their great practical application potential in wastewater remediation.

摘要

同时捕获有机污染物和重金属可以大大减少水修复的时间和成本,但目前这仍然是一个巨大的挑战。在此,通过 Sonogashira-Hagihara 反应,将 1,3,5-三乙炔基苯和 1,3,5-三(4-溴苯基)苯合成了两种新型的巯基/甲基巯基功能化多孔芳香骨架作为吸附剂,随后对苯环进行氯甲基化,最后通过 -Cl 基团的亲核取代反应将 -Cl 基团转化为 -SH 和 -SMe。这两种吸附剂通过傅里叶变换红外光谱、能量色散 X 射线光谱、扫描电子显微镜、氮气吸附分析、热重分析和元素分析进行了表征。吸附实验表明,新吸附剂对芳香族污染物和汞(II)(Hg(II))具有高的吸附能力和快速吸附动力学。两种新吸附剂对甲苯和间二甲苯的最大吸附容量(Q)分别为 531.9-571.4 mg/g,动力学结合速率常数(k)分别为 0.00276-0.02422 g/mg/min,Hg(II)的 Q 值分别为 148.1-180.3 mg/g,k 值分别为 0.00592-0.01573 g/mg/min。此外,新吸附剂对这些污染物具有较高的同时吸附能力,且具有良好的可重复使用性,最后成功应用于高浓度和低浓度两种模拟废水中这些污染物的同时修复,表明其在废水修复中具有很大的实际应用潜力。

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