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Selective separation of Pu(IV) and U(VI) with bisdiglycolamde ligands: solvent extraction and DFT calculations

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Abstract

The extractant tri-n-butyl phosphate (TBP) was used for the separation of Pu(IV) and U(VI) in the PUREX process, which brings phosphorus pollution problems. The ligands in accordance with the “CHON” principle will be helpful to reduce environmental pollution and pressure of subsequent waste treatment. In this work, three environmentally friendly BisDGA ligands in accordance with the “CHON” principle were used for the selective extraction Pu(IV) form U(VI) in 1-octanol system. These ligands showed highly extraction ability for Pu(IV), but hardly extracted U(VI) even under high acidity, which proves that the applicability of these extraction systems for selective separation of Pu(IV) from U(VI). The coordination chemistry of Pu(IV) by slope analyses confirmed that the ligands generated both M:L = 1:1 complexes with Pu(IV). The properties and thermodynamics of the PuL(NO3)4 complexes formed with Pu(IV) and BisDGA ligands were also investigated with the density functional theory (DFT) calculations, and the results verified the relevant experimental conclusion that the affinity of THi-PE-BisDGA for Pu(IV) is better than the other two ligands.

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Acknowledgements

This work was supported by the National Natural Science Foundation of China (Grants 22266001and 22276175) and the Jiangxi Provincial Natural Science Foundation (Grant 20224BAB203007).

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Authors and Affiliations

  1. School of Nuclear Science and Technology, East China University of Technology, Nanchang, 330013, Jiangxi, China

    Hao-Liang Chen, Bin Zhou, Yao Zou & Peng Ren

  2. School of Physics, Nanjing University, Nanjing, 210008, China

    Ming Qi

  3. Sichuan Environmental Protection Engineering Co., Ltd, CNNC, Guangyuan, 628000, China

    Hua-Wu Pei

  4. Zhejiang University of Water Resources and Electric Power, Hangzhou, 310018, China

    Ping-Wen Huang

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Chen, HL., Zhou, B., Qi, M. et al. Selective separation of Pu(IV) and U(VI) with bisdiglycolamde ligands: solvent extraction and DFT calculations. J Radioanal Nucl Chem 332, 3361–3369 (2023). https://doi.org/10.1007/s10967-023-09005-0

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