Crystallization Behavior and Anti-Leaching Performance of Iron Phosphate Glass Solidified Wasteforms Containing Ca3(PO4)2 Simulated Waste
Radioactive TBP/OK organic liquid waste is generated during the processes of uranium purification and spent fuel reprocessing. After high-temperature oxidation treatment, the main products of this waste liquid are calcium phosphate and pyrophosphate. The waste also contains volatile radioactive nucl...
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Editorial Office of Journal of Nuclear and Radiochemistry
2025-04-01
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| Series: | He huaxue yu fangshe huaxue |
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| author | Lin ZHANG Jiong CHANG Ming-shuai YANG Jia-teng WANG Sheng-heng TAN Hui HE |
| author_facet | Lin ZHANG Jiong CHANG Ming-shuai YANG Jia-teng WANG Sheng-heng TAN Hui HE |
| author_sort | Lin ZHANG |
| collection | DOAJ |
| description | Radioactive TBP/OK organic liquid waste is generated during the processes of uranium purification and spent fuel reprocessing. After high-temperature oxidation treatment, the main products of this waste liquid are calcium phosphate and pyrophosphate. The waste also contains volatile radioactive nuclides such as cesium, as well as alpha-emitting nuclides like uranium(U) and plutonium(Pu). If discharged directly or improperly treated, this waste liquid may cause radioactive environmental pollution, which can severely impact ecological health and human health. Therefore, it is essential to use appropriate methods to solidify the cracked products to safely manage and dispose of the secondary waste generated from TBP cracking. Borosilicate glass shows limited tolerance for waste containing large amounts of phosphates, iron oxides, and some heavy metal nuclides(such as La, U, and Bi). In recent years, iron phosphate glass has attracted widespread attention and in-depth research due to its good tolerance for phosphates, sulfates, iron oxides, and other heavy metal elements in high-level radioactive waste, as well as its good stability. The O-P-O bonds in the structure of iron phosphate glass are replaced by more stable Fe-P-O bonds, resulting in a large number of stable Fe-P-O bonds in the glass. Additionally, iron phosphate glass has a lower melting temperature. In this study, a quaternary iron phosphate glass with the composition (37−x)(mole fraction, %, the same below)Fe2O3-xB2O3-56P2O5-7Na2O was used as the vitrification matrix to conduct glass solidification experiments on simulated waste. The experiments investigated the effects of different simulated waste contents and varying B2O3 contents on the crystallization behavior and chemical stability of the iron phosphate glass solidified bodies. Through comprehensive analysis using X-ray diffraction(XRD), differential thermal analysis, and scanning electron microscopy-energy dispersive X-ray spectroscopy(SEM-EDS), it was found that this formulation can tolerate up to 35%(mass fraction, the same below) of waste. The results show that in the (37−x)Fe2O3-xB2O3-56P2O5-7Na2O, when the B2O3 mole fraction is between 0 and 3%, the glass solidified bodies exhibit significantly worse crystallization tendency, density, homogeneity of the glass phase, and leaching of related elements compared to those with a B2O3 mole fraction of 5% to 10%. The PCT-B leaching test results indicate that when the waste loading is 30%, as the B2O3 mole fraction increases, the normalized quality losses of P, B, Cs, Na, and Ca are on the order of 10−5 g/m2; the normalized quality losses of Sr is on the order of 10−6 g/m2; and the normalized quality losses of La is on the order of 10−7 g/m2. The normalized quality losses relationship is as follows: NLP, B, Cs, Na, Ca\begin{document}$\gg $\end{document}NLSr\begin{document}$\gg $\end{document}NLLa\begin{document}$\gg $\end{document}NLFe. The normalized quality losses of all elements are less than 10−2 g/m2. Moreover, as the B content in the system increases, both the glass transition temperature(Tg) and the liquidus temperature(Tc) show an upward trend, indicating that the glass structure is enhanced, the density is increased, and the chemical stability is improved. Therefore, this formulation can be used as a suitable glass solidification formulation for simulated oxide products. |
| format | Article |
| id | doaj-art-b0b5dc14ffd8414184ef7d1a3a4f7055 |
| institution | DOAJ |
| issn | 0253-9950 |
| language | zho |
| publishDate | 2025-04-01 |
| publisher | Editorial Office of Journal of Nuclear and Radiochemistry |
| record_format | Article |
| series | He huaxue yu fangshe huaxue |
| spelling | doaj-art-b0b5dc14ffd8414184ef7d1a3a4f70552025-08-20T03:14:19ZzhoEditorial Office of Journal of Nuclear and RadiochemistryHe huaxue yu fangshe huaxue0253-99502025-04-0147213314110.7538/hhx.2025.47.02.01332024-044Crystallization Behavior and Anti-Leaching Performance of Iron Phosphate Glass Solidified Wasteforms Containing Ca3(PO4)2 Simulated WasteLin ZHANG0Jiong CHANG1Ming-shuai YANG2Jia-teng WANG3Sheng-heng TAN4Hui HE5Department of Radiochemistry, China Institute of Atomic Energy, Beijing 102413, ChinaDepartment of Radiochemistry, China Institute of Atomic Energy, Beijing 102413, ChinaDepartment of Radiochemistry, China Institute of Atomic Energy, Beijing 102413, ChinaDepartment of Radiochemistry, China Institute of Atomic Energy, Beijing 102413, ChinaDepartment of Radiochemistry, China Institute of Atomic Energy, Beijing 102413, ChinaDepartment of Radiochemistry, China Institute of Atomic Energy, Beijing 102413, ChinaRadioactive TBP/OK organic liquid waste is generated during the processes of uranium purification and spent fuel reprocessing. After high-temperature oxidation treatment, the main products of this waste liquid are calcium phosphate and pyrophosphate. The waste also contains volatile radioactive nuclides such as cesium, as well as alpha-emitting nuclides like uranium(U) and plutonium(Pu). If discharged directly or improperly treated, this waste liquid may cause radioactive environmental pollution, which can severely impact ecological health and human health. Therefore, it is essential to use appropriate methods to solidify the cracked products to safely manage and dispose of the secondary waste generated from TBP cracking. Borosilicate glass shows limited tolerance for waste containing large amounts of phosphates, iron oxides, and some heavy metal nuclides(such as La, U, and Bi). In recent years, iron phosphate glass has attracted widespread attention and in-depth research due to its good tolerance for phosphates, sulfates, iron oxides, and other heavy metal elements in high-level radioactive waste, as well as its good stability. The O-P-O bonds in the structure of iron phosphate glass are replaced by more stable Fe-P-O bonds, resulting in a large number of stable Fe-P-O bonds in the glass. Additionally, iron phosphate glass has a lower melting temperature. In this study, a quaternary iron phosphate glass with the composition (37−x)(mole fraction, %, the same below)Fe2O3-xB2O3-56P2O5-7Na2O was used as the vitrification matrix to conduct glass solidification experiments on simulated waste. The experiments investigated the effects of different simulated waste contents and varying B2O3 contents on the crystallization behavior and chemical stability of the iron phosphate glass solidified bodies. Through comprehensive analysis using X-ray diffraction(XRD), differential thermal analysis, and scanning electron microscopy-energy dispersive X-ray spectroscopy(SEM-EDS), it was found that this formulation can tolerate up to 35%(mass fraction, the same below) of waste. The results show that in the (37−x)Fe2O3-xB2O3-56P2O5-7Na2O, when the B2O3 mole fraction is between 0 and 3%, the glass solidified bodies exhibit significantly worse crystallization tendency, density, homogeneity of the glass phase, and leaching of related elements compared to those with a B2O3 mole fraction of 5% to 10%. The PCT-B leaching test results indicate that when the waste loading is 30%, as the B2O3 mole fraction increases, the normalized quality losses of P, B, Cs, Na, and Ca are on the order of 10−5 g/m2; the normalized quality losses of Sr is on the order of 10−6 g/m2; and the normalized quality losses of La is on the order of 10−7 g/m2. The normalized quality losses relationship is as follows: NLP, B, Cs, Na, Ca\begin{document}$\gg $\end{document}NLSr\begin{document}$\gg $\end{document}NLLa\begin{document}$\gg $\end{document}NLFe. The normalized quality losses of all elements are less than 10−2 g/m2. Moreover, as the B content in the system increases, both the glass transition temperature(Tg) and the liquidus temperature(Tc) show an upward trend, indicating that the glass structure is enhanced, the density is increased, and the chemical stability is improved. Therefore, this formulation can be used as a suitable glass solidification formulation for simulated oxide products.https://jnrc.xml-journal.net/cn/article/doi/10.7538/hhx.2025.47.02.0133iron phosphate glassvitrificationintermediate to high-level radioactive waste |
| spellingShingle | Lin ZHANG Jiong CHANG Ming-shuai YANG Jia-teng WANG Sheng-heng TAN Hui HE Crystallization Behavior and Anti-Leaching Performance of Iron Phosphate Glass Solidified Wasteforms Containing Ca3(PO4)2 Simulated Waste He huaxue yu fangshe huaxue iron phosphate glass vitrification intermediate to high-level radioactive waste |
| title | Crystallization Behavior and Anti-Leaching Performance of Iron Phosphate Glass Solidified Wasteforms Containing Ca3(PO4)2 Simulated Waste |
| title_full | Crystallization Behavior and Anti-Leaching Performance of Iron Phosphate Glass Solidified Wasteforms Containing Ca3(PO4)2 Simulated Waste |
| title_fullStr | Crystallization Behavior and Anti-Leaching Performance of Iron Phosphate Glass Solidified Wasteforms Containing Ca3(PO4)2 Simulated Waste |
| title_full_unstemmed | Crystallization Behavior and Anti-Leaching Performance of Iron Phosphate Glass Solidified Wasteforms Containing Ca3(PO4)2 Simulated Waste |
| title_short | Crystallization Behavior and Anti-Leaching Performance of Iron Phosphate Glass Solidified Wasteforms Containing Ca3(PO4)2 Simulated Waste |
| title_sort | crystallization behavior and anti leaching performance of iron phosphate glass solidified wasteforms containing ca3 po4 2 simulated waste |
| topic | iron phosphate glass vitrification intermediate to high-level radioactive waste |
| url | https://jnrc.xml-journal.net/cn/article/doi/10.7538/hhx.2025.47.02.0133 |
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