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基于金属有机骨架的耐辐照富氧离子阱高效捕获 Th(IV)和 U(VI)。

Efficient Capture of Th(IV) and U(VI) by Radiation-Resistant Oxygen-Rich Ion Traps Based on a Metal-Organic Framework.

机构信息

State Key Laboratory of Organic-Inorganic Composites, College of Chemical Engineering, Beijing University of Chemical Technology, Beijing 100029, China.

Department of Radiochemistry, China Institute of Atomic Energy, Beijing 102413, China.

出版信息

ACS Appl Mater Interfaces. 2023 May 24;15(20):25029-25040. doi: 10.1021/acsami.3c02582. Epub 2023 May 9.

Abstract

Herein, based on a well-stabilized Ti-MOF (IEF-11), an oxygen-rich ion trap with synergy interaction of active atoms was proposed for the removal of Th(IV) and U(VI) from aqueous solutions. Due to the high coordination number of Ti and compact framework structure, IEF-11 has excellent resistance toward β-ray irradiation, even under 1000 kGy irradiation dosage. Meanwhile, owing to the special chelating effect of the oxygen-rich ion traps, the maximum adsorption amounts of IEF-11 for Th(IV) (pH = 3.0) and U(VI) (pH = 5.0) ions can reach 305.9 and 240.7 mg g, and the separation coefficients exceed 200 for Th(IV)/Nd(III), Th(IV)/Sm(III), and Th(IV)/Eu(III) and 100 for U(VI)/Eu(III), U(VI)/La(III), and U(VI)/Sr(II). Moreover, IEF-11 shows fast adsorption kinetics with an equilibrium time of ∼100 min. The adsorption amount almost remains even after four adsorption-desorption cycles. Finally, experimental and theoretical calculations indicate that Th(IV) and U(VI) ions are anchored in the ion trap in the form of chemical bonds. Meanwhile, the circular pore trap (class I trap) than the long pore trap (class II trap) is considered to be the better adsorption site. We expect that our work will provide a new insight for constructing effective adsorbents for radioactive nuclides.

摘要

在此,基于稳定的 Ti-MOF(IEF-11),提出了一种具有协同作用的富氧离子阱,用于从水溶液中去除 Th(IV) 和 U(VI)。由于 Ti 的高配位数和紧凑的框架结构,IEF-11 具有出色的抗 β 射线辐射能力,即使在 1000 kGy 的辐照剂量下也是如此。同时,由于富氧离子阱的特殊螯合效应,IEF-11 对 Th(IV)(pH = 3.0)和 U(VI)(pH = 5.0)离子的最大吸附量分别可达 305.9 和 240.7 mg g-1,分离系数超过 200,如 Th(IV)/Nd(III)、Th(IV)/Sm(III) 和 Th(IV)/Eu(III),以及 100,如 U(VI)/Eu(III)、U(VI)/La(III) 和 U(VI)/Sr(II)。此外,IEF-11 具有快速的吸附动力学,平衡时间约为 100 min。经过四次吸附-解吸循环后,吸附量几乎保持不变。最后,实验和理论计算表明,Th(IV)和 U(VI)离子以化学键的形式锚定在离子阱中。同时,认为环状孔阱(I 类阱)比长孔阱(II 类阱)是更好的吸附位点。我们希望我们的工作将为构建放射性核素的有效吸附剂提供新的思路。

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