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多功能交联合成 EDTA 修饰的 UiO-66-NH/棉织物复合材料,用于同时捕获重金属和染料以及高效降解有机磷。

Versatile crosslinking synthesis of an EDTA-modified UiO-66-NH/cotton fabric composite for simultaneous capture of heavy metals and dyes and efficient degradation of organophosphate.

机构信息

Shandong Provincial Key Laboratory of Water Pollution Control and Resource Reuse, School of Environmental Science and Engineering, Shandong University, Qingdao, 266000, China.

Hubei Key Laboratory of Biomass Fibers and Eco-dyeing & Finishing, School of Chemistry and Chemical Engineering, Wuhan Textile University, Wuhan, 430073, China; School of Chemistry and Chemical Engineering, Jiangxi Science and Technology Normal University, Nanchang, 330013, China.

出版信息

Environ Pollut. 2023 Jan 1;316(Pt 2):120622. doi: 10.1016/j.envpol.2022.120622. Epub 2022 Nov 9.

Abstract

The metal-organic frameworks/cotton fabric composites (MOFs/CFCs) have emerged as a new type of prospective materials for environmental cleanup, due to their convenient recyclability and high removal efficiency towards hazardous pollutants. However, their practical applications are limited by complicated synthetic conditions, insufficient interface bonding and poor adsorption capacity. Herein, for the first time, a robust ethylenediaminetetraacetic acid (EDTA)-functionalized MOFs/CFC is prepared based on UiO-66-NH crystals by using EDTA dianhydride as the cross-linking agent, and applied for simultaneous removal of heavy metals and dyes, as well as degradation of chemical warfare agents. The as-prepared EDTA-UiO-66-NH/CFC shows extraordinary monocomponent adsorption performance with maximum adsorption capacity of 158.7, 126.2, 131.5, 117.4 and 104.5 mg/g for Cd(II), Cu(II), methylene blue, crystal violet and safranin O, respectively. Interestingly, in metal-dyes binary system, the uptake of Cu(II) by EDTA-UiO-66-NH/CFC increases significantly when co-existing high concentration of dyes. The results indicate that the synergistic and simultaneous removal of both dyes and metal from complex systems can be realized by EDTA-UiO-66-NH/CFC via multiple mechanisms. The EDTA-UiO-66-NH/CFC also exhibits an outstanding catalytic performance for degrading dimethyl 4-nitrophenylphosphate. Besides, it can be reused for several times without obvious decrease of its adsorption and catalysis efficiencies. More impressively, the cross-linking reaction approach can not only anchor UiO-66-NH crystals firmly onto cotton fabric, but also facilitate in-situ formation of abundant adsorption sties on the adsorbent surface. Therefore, this work offers a simple and versatile synthetic strategy to develop high-performance environmental material for multiple pollutants remediation.

摘要

金属-有机骨架/棉织物复合材料(MOFs/CFCs)由于其方便的可回收性和对危险污染物的高去除效率,已成为环境净化的新型有前途的材料。然而,其实际应用受到复杂的合成条件、界面结合不充分和吸附容量低的限制。在此,首次使用乙二胺四乙酸二酐(EDTA 二酐)作为交联剂,基于 UiO-66-NH 晶体制备了一种坚固的乙二胺四乙酸(EDTA)功能化 MOFs/CFC,并将其应用于同时去除重金属和染料以及化学战剂的降解。所制备的 EDTA-UiO-66-NH/CFC 表现出非凡的单一组分吸附性能,对 Cd(II)、Cu(II)、亚甲基蓝、结晶紫和藏红 O 的最大吸附容量分别为 158.7、126.2、131.5、117.4 和 104.5 mg/g。有趣的是,在金属-染料二元体系中,当共存高浓度染料时,EDTA-UiO-66-NH/CFC 对 Cu(II)的吸收显著增加。结果表明,通过 EDTA-UiO-66-NH/CFC 可以通过多种机制实现从复杂体系中协同和同时去除染料和金属。EDTA-UiO-66-NH/CFC 还对二甲氨基 4-硝基苯膦酸酯的降解表现出出色的催化性能。此外,它可以重复使用几次而不会明显降低其吸附和催化效率。更令人印象深刻的是,交联反应方法不仅可以将 UiO-66-NH 晶体牢固地固定在棉织物上,而且还可以促进在吸附剂表面原位形成丰富的吸附位点。因此,这项工作为开发用于多种污染物修复的高性能环境材料提供了一种简单而通用的合成策略。

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