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壳聚糖/单宁酸固化及官能团改性对Cu-MOF吸附五种废水中铀的增强机制

Enhancement mechanism of chitosan/tannic acid curing and functional group modification on uranium adsorption in five types of wastewater by Cu-MOF.

作者信息

Huang Yulin, Wang Qingliang, Xin Qi, Lei Zhiwu, Hu Eming, Li Le, Liang Feng, Wang Hongqiang

机构信息

School of Resource & Environment and Safety Engineering, University of South China, Hengyang 421001, China.

School of Public Health, University of South China, Hengyang 421001, China.

出版信息

J Hazard Mater. 2025 Jul 15;492:138185. doi: 10.1016/j.jhazmat.2025.138185. Epub 2025 Apr 7.

DOI:10.1016/j.jhazmat.2025.138185
PMID:40209408
Abstract

To advance the application of Cu-metal-organic framework (Cu-MOF) in uranium wastewater treatment for the nuclear industry, it is essential to address the limitations of its powder form and rigid structure while enhancing its adsorption capacity. In this study, a Cu-MOF@CSTA composite adsorbent was synthesized by solidifying Cu-MOF with chitosan/tannic acid and modifying its functional groups to improve uranium adsorption performance. The U(VI) theoretical maximum adsorption capacity of Cu-MOF@CSTA at 288 K (pH = 5) was 2507.73 mg/g, and the adsorption process was characterized as a spontaneous exothermic reaction. The uranium removal rate in mine wastewater (pore water and seepage water) reached 100 %. Uranium removal efficiencies in wastewater containing 100 mg/L fluoride ions, ammonia ions, and urea were remarkably high at 99.34 %, 99.63 %, and 98.94 %, respectively, demonstrating the composite adsorbent's robust anti-jamming capability. Mechanistic analysis revealed that the synergistic effects of hydroxyl, amino, and sulfur functional groups on the Cu-MOF@CSTA surface facilitated uranium adsorption. Competitive adsorption experiments confirmed that Cu-MOF@CSTA exhibits excellent selectivity for uranium. The chitosan, solidified by tannic acid as a flexible carrier, stabilized the Cu-MOF, highlighting its significant potential for uranium adsorption in wastewater treatment applications.

摘要

为了推动铜基金属有机框架(Cu-MOF)在核工业铀废水处理中的应用,在提高其吸附能力的同时,解决其粉末形式和刚性结构的局限性至关重要。在本研究中,通过用壳聚糖/单宁酸固化Cu-MOF并修饰其官能团以提高铀吸附性能,合成了一种Cu-MOF@CSTA复合吸附剂。Cu-MOF@CSTA在288K(pH = 5)下对U(VI)的理论最大吸附容量为2507.73mg/g,吸附过程为自发放热反应。矿井废水(孔隙水和渗流水)中的铀去除率达到100%。在含有100mg/L氟离子、铵离子和尿素的废水中,铀去除效率分别高达99.34%、99.63%和98.94%,表明该复合吸附剂具有强大的抗干扰能力。机理分析表明,Cu-MOF@CSTA表面的羟基、氨基和硫官能团的协同作用促进了铀的吸附。竞争吸附实验证实,Cu-MOF@CSTA对铀具有优异的选择性。由单宁酸固化的壳聚糖作为柔性载体,稳定了Cu-MOF,突出了其在废水处理应用中吸附铀的巨大潜力。

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