丙二酸存在下氧化气氛生成的U3O8、FeUO4和uo2 - zr -不锈钢体系样品的溶解行为

IF 3.2 2区 工程技术 Q3 MATERIALS SCIENCE, MULTIDISCIPLINARY Journal of Nuclear Materials Pub Date : 2025-02-01 Epub Date: 2024-12-07 DOI:10.1016/j.jnucmat.2024.155561
Ryutaro Tonna , Takayuki Sasaki , Yoshihiro Okamoto , Taishi Kobayashi
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引用次数: 0

摘要

了解uo2 - zr -不锈钢(SS)体系在有机酸存在下的溶解行为,对于福岛第一核电站的安全退役,以及未来对燃料碎片深层地质处置的处理至关重要。通过丙二酸静态浸出试验,研究了氧化条件下加热的UO2-Zr-SS样品的溶解行为,以及样品中形成的单一铀相(U3O8和FeUO4)。丙二酸通过络合物的形成促进了U3O8和FeUO4固相的溶解。U3O8和FeUO4的铀浓度随丙二酸浓度的增加而增加,并在稳定状态下匹配。在没有丙二酸的情况下,由于铀在铁水解固相上的吸附作用,FeUO4的U浓度小于其溶解度。UO2-Zr-SS体系样品长时间浸渍后的铀浓度可以用U3O8和FeUO4的行为来解释。在没有丙二酸的情况下,U的浓度由于吸附在铁固相上而降低,类似于FeUO4的行为。相反,在丙二酸存在下,U浓度与U3O8和FeUO4的浓度一致。
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Dissolution behavior of U3O8, FeUO4, and UO2-Zr-stainless steel system samples generated in an oxidative atmosphere in the presence of malonic acid
Understanding the dissolution behavior of the UO2-Zr-stainless steel (SS) system in the presence of organic acids is crucial for the safe decommissioning of the Fukushima Daiichi Nuclear Power Plants, as well as for the future treatment toward deep geological disposal of fuel debris. The dissolution behavior of UO2-Zr-SS samples heated under oxidative conditions, along with the single uranium phases formed in the samples (U3O8 and FeUO4), was investigated through static leaching tests using malonic acid. Malonic acid promoted the dissolution of both U3O8 and FeUO4 solid phases owing to complex formation. The uranium concentrations of U3O8 and FeUO4 increased with malonic acid concentration and matched at steady state. In the absence of malonic acid, the U concentration of FeUO4 was less than its solubility because of uranium adsorption on an iron hydrolysis solid phase. The uranium concentration after long immersion of the UO2-Zr-SS system samples could be explained by the behavior of U3O8 and FeUO4. In the absence of malonic acid, U concentration decreased owing to adsorption onto the iron solid phase, similar to the behavior of FeUO4. In contrast, in the presence of malonic acid, U concentration was consistent with that observed for U3O8 and FeUO4.
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来源期刊
Journal of Nuclear Materials
Journal of Nuclear Materials 工程技术-材料科学:综合
CiteScore
5.70
自引率
25.80%
发文量
601
审稿时长
63 days
期刊介绍: The Journal of Nuclear Materials publishes high quality papers in materials research for nuclear applications, primarily fission reactors, fusion reactors, and similar environments including radiation areas of charged particle accelerators. Both original research and critical review papers covering experimental, theoretical, and computational aspects of either fundamental or applied nature are welcome. The breadth of the field is such that a wide range of processes and properties in the field of materials science and engineering is of interest to the readership, spanning atom-scale processes, microstructures, thermodynamics, mechanical properties, physical properties, and corrosion, for example. Topics covered by JNM Fission reactor materials, including fuels, cladding, core structures, pressure vessels, coolant interactions with materials, moderator and control components, fission product behavior. Materials aspects of the entire fuel cycle. Materials aspects of the actinides and their compounds. Performance of nuclear waste materials; materials aspects of the immobilization of wastes. Fusion reactor materials, including first walls, blankets, insulators and magnets. Neutron and charged particle radiation effects in materials, including defects, transmutations, microstructures, phase changes and macroscopic properties. Interaction of plasmas, ion beams, electron beams and electromagnetic radiation with materials relevant to nuclear systems.
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