Exploring constituent redistribution in irradiated U-19Pu-14Zr fuel via electron probe microanalysis

IF 2.8 2区工程技术 Q3 MATERIALS SCIENCE, MULTIDISCIPLINARY Journal of Nuclear Materials Pub Date : 2024-09-17 DOI:10.1016/j.jnucmat.2024.155411

Karen E. Wright , Lindsey Lecrivain , Cortney Pincock , Magen Coleman , Pamela Wiscaver , Beau Barker , Luiza Gimenes Rodrigues Albuquerque , Luca Capriotti , Assel Aitkaliyeva

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Abstract

The phenomena of constituent redistribution, wherein a previously homogeneous metallic fuel forms discrete, radially concentric compositional zones upon irradiation was investigated by examining an irradiated U-19Pu-14Zr fuel (where numbers represent wt. %) with a burnup of 11.5 at.% with electron probe microanalysis (EPMA) and quadruple inductively coupled plasma mass spectroscopy (Q-ICP-MS).

EPMA-generated U, Pu, and Zr compositional data obtained from a diameter traverse of the sample was converted to mass and was used to: 1) compare the overall fuel element analysis results between the two methods, 2) determine the number of compositionally distinct zones forming as a result of constituent redistribution; and 3) quantify the post-irradiation loss or gain of U, Pu, and Zr atoms in each distinct compositional zone.

Weight percent concentrations of U, Pu, and Zr for the overall cross section compare favorably between the two analytical methods, suggesting that the spatially resolved EPMA analysis complements bulk chemical analysis.

Among the four identified compositional zones, post-irradiation quantification of U, Pu, and Zr elemental atom content changes shows that the quantity of U atoms lost from the innermost zone is slightly less than the quantity of U atoms gained by the middle two zones, and the quantity of Zr atoms lost from the high-U third zone is slightly less than is gained by the two innermost zones. Pu is lost from all four zones, although the innermost zone and the high-U third zone lose a significantly higher percentage (> 22 %) of their initial Pu atoms than the other two zones. For all three elements, EPMA cannot distinguish between atoms lost due to transport to a different zone from atoms lost due to nuclear processes; however, the insight gained from using this process can be used to experiment with new modeling techniques to predict constituent redistribution in U-Pu-Zr fuels.

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通过电子探针显微分析探索辐照 U-19Pu-14Zr 燃料中的成分再分布

通过使用电子探针显微分析（EPMA）和四重电感耦合等离子体质谱（Q-ICP-MS）对燃烧度为 11.5 at.%、经过辐照的 U-19Pu-14Zr 燃料（数字代表重量百分比）进行检测，研究了成分再分布现象，即之前均匀的金属燃料在辐照后形成离散的、径向同心的成分区。电子探针显微分析（EPMA）和四重电感耦合等离子体质谱（Q-ICP-MS）对燃烧度为 11.5 at.% 的辐照铀-19Pu-14Zr 燃料（数字代表重量百分比）进行了研究：1) 比较两种方法的总体燃料元素分析结果；2) 确定由于成分再分布而形成的不同成分区的数量；3) 量化每个不同成分区中辐照后铀、钚和锆原子的损耗或增益。在已确定的四个成分区中，对辐照后铀、钚和锆元素原子含量变化的定量分析表明，最内层区损失的铀原子数量略少于中间两个区获得的铀原子数量，而高铀第三区损失的锆原子数量略少于最内层两个区获得的锆原子数量。所有四个区都损失了钚，但最内区和高铀第三区损失的钚原子占其初始钚原子的百分比（22%）明显高于其他两个区。对于所有这三种元素，EPMA 无法区分因迁移到不同区域而损失的原子和因核过程而损失的原子；不过，利用这一过程获得的洞察力可用于试验新的建模技术，以预测铀-钚-锌燃料中的成分再分布。

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来源期刊

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.