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多官能团 MOF@COF 复合材料的合理设计用于增强从水溶液中去除 U(VI)。

Rational design of MOF@COF composites with multi-site functional groups for enhanced elimination of U(VI) from aqueous solution.

机构信息

MOE Key Laboratory of Resources and Environmental Systems Optimization, College of Environmental Science and Engineering, North China Electric Power University, Beijing, 102206, PR China.

Hebei Key Lab of Power Plant Flue Gas Multi-Pollutants Control, Department of Environmental Science and Engineering, North China Electric Power University, Baoding, 071003, PR China.

出版信息

Chemosphere. 2023 Nov;341:140086. doi: 10.1016/j.chemosphere.2023.140086. Epub 2023 Sep 5.

DOI:10.1016/j.chemosphere.2023.140086
PMID:37678593
Abstract

Both environment and human beings were menaced by the widespread application of radioactive uranium, high-performance and effective elimination of uranium from wastewater is of important meaning for development of environmental sustainability in the future. In this study, the water-stable MOF material and the highly crystalline COF were compounded by a mild hydrothermal strategy, which achieved efficient removal of U(VI) through the synergistic effect. The composites showed the characteristics of both COFs and MOFs, which will possess higher stability, larger surface area and faster adsorption efficiency that cannot be carried out by a single component. Batch experiments and characterizations (SEM, TEM, XRD, FT-IR, BET, XPS, etc.) indicated that UiO-66-NH@LZU1 had more stable and multi-layer pore structure and rich active functional groups. The Langmuir model and the pseudo-second-order kinetics fitting was more suitable for the U(VI) elimination process. The greatest uranium adsorbing capacity of UiO-66-NH@LZU1 (180.4 mg g) was observed to exceed the UiO-66-NH (108.8 mg g) and COF-LZU1 (65.8 mg g), which reached the excellent hybrid effects. Furthermore, FT-IR and XPS analyses confirmed that the most nitrogen-containing group from COF-LZU1 and oxygen-containing group of UiO-66-NH could be combined with U(VI). In addition, electrostatic interaction was also a mechanism during the removal process. This work displayed that UiO-66-NH@LZU1 was a prospective hybrid material for radioactive waste remediation. The compound method and application mentioned in this work had provided a theoretical basis for designing and developing multi-functional composite adsorbents, which contributed to the development of new materials for radioactive wastewater treatment technologies.

摘要

广泛应用放射性铀对环境和人类都构成了威胁,从废水中高效、有效地去除铀对于未来环境可持续性的发展具有重要意义。在这项研究中,采用温和的水热策略将水稳定的 MOF 材料和高结晶 COF 复合,通过协同作用实现了 U(VI)的高效去除。复合材料具有 COFs 和 MOFs 的特点,将具有更高的稳定性、更大的表面积和更快的吸附效率,这是单一成分无法实现的。批量实验和表征(SEM、TEM、XRD、FT-IR、BET、XPS 等)表明,UiO-66-NH@LZU1 具有更稳定的多层孔结构和丰富的活性官能团。Langmuir 模型和拟二级动力学拟合更适合 U(VI)的去除过程。UiO-66-NH@LZU1(180.4mg g)的最大铀吸附容量被观察到超过 UiO-66-NH(108.8mg g)和 COF-LZU1(65.8mg g),达到了优异的混合效果。此外,FT-IR 和 XPS 分析证实,来自 COF-LZU1 的最多含氮基团和 UiO-66-NH 的含氧基团可以与 U(VI)结合。此外,静电相互作用也是去除过程中的一种机制。这项工作表明,UiO-66-NH@LZU1 是一种有前途的放射性废物修复用混合材料。本工作中提到的复合方法和应用为设计和开发多功能复合吸附剂提供了理论依据,为放射性废水处理技术的新材料发展做出了贡献。

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