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二维铜基金属-有机骨架纳米片复合材料:一步合成及高效 U(VI)固定。

Two-dimensional copper-based metal-organic frameworks nano-sheets composites: One-step synthesis and highly efficient U(VI) immobilization.

机构信息

Department of Chemistry and Engineering, Heze University, Heze 274500, PR China; CAS Key Laboratory of Photovoltaic and Energy Conservation Materials, Institute of Plasma Physics, Chinese Academy of Sciences, P.O. Box 1126, Hefei, 230031, PR China.

Department of Chemistry and Engineering, Heze University, Heze 274500, PR China.

出版信息

J Hazard Mater. 2019 Jul 5;373:580-590. doi: 10.1016/j.jhazmat.2019.03.119. Epub 2019 Mar 28.

DOI:10.1016/j.jhazmat.2019.03.119
PMID:30952003
Abstract

In this study, a new kind of thin 2D MOFs nano-sheets (MNS) was successfully prepared through complexation between 2-methylimidazole and Cu(II) by a one-step, and cost-effective route. The structural morphologies can be tuned by adjusting the ratio of MeOH/HO. The synthesized MNS (MNS-1, MNS-2, MNS-3 and MNS-4) were fully characterized and the results indicated that the synthesized MNS were freestanding and possess micro-sized lateral dimensions and nanoscale thickness of sub-25 nm. All the obtained MNS display great performance with the adsorption capacity hierarchy of MNS-2 (591.79 mg·g) > MNS-3 (409.49 mg·g) > MNS-4 (387.07 mg·g) > MNS-1 (384.84 mg·g) at pH ˜ 6.0, and 298 K. The thermodynamic parameters indicated the exothermic and spontaneous nature of U(VI) immobilization. The U(VI) immobilization mechanism was achieved through the complexation between U(VI) and C-N(H) /-OH groups. This work supplies a facile and purposeful approach for developing 2D MOFs nano-sheets toward a highly efficient immobilization of U(VI), and it also promotes the preparation of structure-based design of nanomaterials for radionuclide-containing-medium pretreatment.

摘要

在这项研究中,通过 2-甲基咪唑与 Cu(II) 的一步、经济高效的络合反应,成功制备了一种新型的二维 MOFs 纳米薄片(MNS)。通过调节 MeOH/HO 的比例可以调整结构形态。合成的 MNS(MNS-1、MNS-2、MNS-3 和 MNS-4)进行了充分的表征,结果表明合成的 MNS 是独立的,具有微尺寸的横向尺寸和亚 25nm 的纳米级厚度。所有获得的 MNS 都表现出优异的性能,吸附容量顺序为 MNS-2(591.79mg·g)>MNS-3(409.49mg·g)>MNS-4(387.07mg·g)>MNS-1(384.84mg·g),在 pH ˜ 6.0 和 298 K 下。热力学参数表明 U(VI)固定是放热和自发的。U(VI)的固定机制是通过 U(VI)与 C-N(H)/-OH 基团的络合实现的。这项工作为开发二维 MOFs 纳米薄片提供了一种简便且有针对性的方法,用于高效固定 U(VI),同时也促进了基于结构设计的纳米材料的制备,用于放射性核素含介质的预处理。

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