Performance of Graphene Oxide Membrane for Separating U From U-Nb-Zr Alloys Under Strong Nitric Acid System

There are a large amount of uranium, niobium, and niobium elements in the unqualified products generated during the production and manufacturing process of U-Nb-Zr alloy materials, as well as in the wastewater generated during the analysis and characterization process. In order to achieve the recove...

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Main Authors: Dong-ping ZHANG, Li-qin HUANG, Lei SU, Yuan-ting XIONG, Feng ZHAO, Yue-xiang LU
Format: Article
Language:zho
Published: Editorial Office of Journal of Nuclear and Radiochemistry 2025-06-01
Series:He huaxue yu fangshe huaxue
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Online Access:https://jnrc.xml-journal.net/cn/article/doi/10.7538/hhx.2025.47.03.0224
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author Dong-ping ZHANG
Li-qin HUANG
Lei SU
Yuan-ting XIONG
Feng ZHAO
Yue-xiang LU
author_facet Dong-ping ZHANG
Li-qin HUANG
Lei SU
Yuan-ting XIONG
Feng ZHAO
Yue-xiang LU
author_sort Dong-ping ZHANG
collection DOAJ
description There are a large amount of uranium, niobium, and niobium elements in the unqualified products generated during the production and manufacturing process of U-Nb-Zr alloy materials, as well as in the wastewater generated during the analysis and characterization process. In order to achieve the recovery and reuse of uranium and reduce the discharge of radioactive waste, this work adopted a membrane separation technology based on graphene oxide membranes(GOMs). By utilizing the size difference between uranyl ions and niobium and zirconium hydrate ions, the separation of uranyl ions from uranium, niobium and zirconium ion solutions under strong nitric acid system was explored. Six groups of GOMs with different graphite particle sizes and oxidation degrees were prepared. The effects of membrane oxidation degree, membrane thickness, solution acidity, and ion concentration on screening and separation efficiency was evaluated. SEM show that the thickness of 1.2 mg GOMs is about 1 μm, and there are obvious wrinkles on the surface of GOMs, provided a channel for the passage of small molecules and ions. XPS and FTIR show that the order of oxidation degree of the six groups of GOMs is 325S2>200S2>200S1>325S1>100S1>100S2. The experimental results show that the GOMs products(200S1) with 200 mesh(particle size is 75 μm) graphite as the raw material and oxidized at 35 ℃ for 2 h have smaller interlayer spacing in 3 mol/L HNO3 solution, and this material can most effectively achieve the separation of uranium from niobium and zirconium. Under the screening separation conditions of 200S1 membrane mass of 1.2 mg, solution acidity of 3 mol/L HNO3, \begin{document}${\mathrm{UO}}_2^{2+} $\end{document} initial concentration of 3.7 mmol/L, and Nb5+ and Zr4+ initial concentrations of 1.1 mmol/L, the Nb5+ concentration(0.40 mmol/L) and Zr4+ concentration(0.38 mmol/L) measured in infiltration side at 48 h are approximately twice the concentration of \begin{document}${\mathrm{UO}}_2^{2+} $\end{document}(0.21 mmol/L). The permeability of \begin{document}${\mathrm{UO}}_2^{2+} $\end{document} at 48 h is only 5.32%, while the ion permeability of Nb5+ and Zr4+ are 36.39% and 34.30%, respectively, approaching osmotic equilibrium. The pseudo-first order separation rate constant of Nb5+(0.0087 h−1) is approximately 8 times that of \begin{document}${\mathrm{UO}}_2^{2+} $\end{document}(0.0011 h−1), while Zr4+(0.0080 h−1) is approximately 7 times that of \begin{document}${\mathrm{UO}}_2^{2+} $\end{document}(0.0011 h−1). The separation factors of α(Nb/U) and α(Zr/U) reach 10.2 and 9.3, respectively. In addition, cyclic experiments show that the 200S1 membrane still has screening and separation ability after being reused 5 times. This work provides a new method for the recovery of uranium in U-Nb-Zr materials, and can also provide technical reference for the separation of uranium in high-level radioactive waste.
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spelling doaj-art-5904df2537e94ec9bf80b9eddfd724842025-08-20T03:29:34ZzhoEditorial Office of Journal of Nuclear and RadiochemistryHe huaxue yu fangshe huaxue0253-99502025-06-0147322423410.7538/hhx.2025.47.03.02242024-059Performance of Graphene Oxide Membrane for Separating U From U-Nb-Zr Alloys Under Strong Nitric Acid SystemDong-ping ZHANG0Li-qin HUANG1Lei SU2Yuan-ting XIONG3Feng ZHAO4Yue-xiang LU5National Key Laboratory of Advanced Nuclear Energy Technology, Nuclear Power Institute of China, Chengdu 610213, ChinaInstitute of Nuclear and New Energy Technology, Tsinghua University, Beijing 100084, ChinaNational Key Laboratory of Advanced Nuclear Energy Technology, Nuclear Power Institute of China, Chengdu 610213, ChinaNational Key Laboratory of Advanced Nuclear Energy Technology, Nuclear Power Institute of China, Chengdu 610213, ChinaNational Key Laboratory of Advanced Nuclear Energy Technology, Nuclear Power Institute of China, Chengdu 610213, ChinaInstitute of Nuclear and New Energy Technology, Tsinghua University, Beijing 100084, ChinaThere are a large amount of uranium, niobium, and niobium elements in the unqualified products generated during the production and manufacturing process of U-Nb-Zr alloy materials, as well as in the wastewater generated during the analysis and characterization process. In order to achieve the recovery and reuse of uranium and reduce the discharge of radioactive waste, this work adopted a membrane separation technology based on graphene oxide membranes(GOMs). By utilizing the size difference between uranyl ions and niobium and zirconium hydrate ions, the separation of uranyl ions from uranium, niobium and zirconium ion solutions under strong nitric acid system was explored. Six groups of GOMs with different graphite particle sizes and oxidation degrees were prepared. The effects of membrane oxidation degree, membrane thickness, solution acidity, and ion concentration on screening and separation efficiency was evaluated. SEM show that the thickness of 1.2 mg GOMs is about 1 μm, and there are obvious wrinkles on the surface of GOMs, provided a channel for the passage of small molecules and ions. XPS and FTIR show that the order of oxidation degree of the six groups of GOMs is 325S2>200S2>200S1>325S1>100S1>100S2. The experimental results show that the GOMs products(200S1) with 200 mesh(particle size is 75 μm) graphite as the raw material and oxidized at 35 ℃ for 2 h have smaller interlayer spacing in 3 mol/L HNO3 solution, and this material can most effectively achieve the separation of uranium from niobium and zirconium. Under the screening separation conditions of 200S1 membrane mass of 1.2 mg, solution acidity of 3 mol/L HNO3, \begin{document}${\mathrm{UO}}_2^{2+} $\end{document} initial concentration of 3.7 mmol/L, and Nb5+ and Zr4+ initial concentrations of 1.1 mmol/L, the Nb5+ concentration(0.40 mmol/L) and Zr4+ concentration(0.38 mmol/L) measured in infiltration side at 48 h are approximately twice the concentration of \begin{document}${\mathrm{UO}}_2^{2+} $\end{document}(0.21 mmol/L). The permeability of \begin{document}${\mathrm{UO}}_2^{2+} $\end{document} at 48 h is only 5.32%, while the ion permeability of Nb5+ and Zr4+ are 36.39% and 34.30%, respectively, approaching osmotic equilibrium. The pseudo-first order separation rate constant of Nb5+(0.0087 h−1) is approximately 8 times that of \begin{document}${\mathrm{UO}}_2^{2+} $\end{document}(0.0011 h−1), while Zr4+(0.0080 h−1) is approximately 7 times that of \begin{document}${\mathrm{UO}}_2^{2+} $\end{document}(0.0011 h−1). The separation factors of α(Nb/U) and α(Zr/U) reach 10.2 and 9.3, respectively. In addition, cyclic experiments show that the 200S1 membrane still has screening and separation ability after being reused 5 times. This work provides a new method for the recovery of uranium in U-Nb-Zr materials, and can also provide technical reference for the separation of uranium in high-level radioactive waste.https://jnrc.xml-journal.net/cn/article/doi/10.7538/hhx.2025.47.03.0224graphene oxide membraneuraniumniobiumzirconiumsieving
spellingShingle Dong-ping ZHANG
Li-qin HUANG
Lei SU
Yuan-ting XIONG
Feng ZHAO
Yue-xiang LU
Performance of Graphene Oxide Membrane for Separating U From U-Nb-Zr Alloys Under Strong Nitric Acid System
He huaxue yu fangshe huaxue
graphene oxide membrane
uranium
niobium
zirconium
sieving
title Performance of Graphene Oxide Membrane for Separating U From U-Nb-Zr Alloys Under Strong Nitric Acid System
title_full Performance of Graphene Oxide Membrane for Separating U From U-Nb-Zr Alloys Under Strong Nitric Acid System
title_fullStr Performance of Graphene Oxide Membrane for Separating U From U-Nb-Zr Alloys Under Strong Nitric Acid System
title_full_unstemmed Performance of Graphene Oxide Membrane for Separating U From U-Nb-Zr Alloys Under Strong Nitric Acid System
title_short Performance of Graphene Oxide Membrane for Separating U From U-Nb-Zr Alloys Under Strong Nitric Acid System
title_sort performance of graphene oxide membrane for separating u from u nb zr alloys under strong nitric acid system
topic graphene oxide membrane
uranium
niobium
zirconium
sieving
url https://jnrc.xml-journal.net/cn/article/doi/10.7538/hhx.2025.47.03.0224
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