Fission product solubility and speciation in UN SIMFUEL

IF 2.8 2区工程技术 Q3 MATERIALS SCIENCE, MULTIDISCIPLINARY

Journal of Nuclear Materials Pub Date : 2025-04-09 DOI:10.1016/j.jnucmat.2025.155815

J.H. Stansby , D.A. Lopes , F. Sweidan , Y. Mishchenko , M. Ranger , M. Jolkkonen , V.K. Peterson , E.G. Obbard , P. Olsson

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Abstract

U(X)N-based SIMFUEL samples, where X represents Zr, Nb, Mo, and Ru, were fabricated using spark plasma sintering. These samples were characterized by neutron diffraction and scanning electron microscopy to gain insights into fission product solubility and speciation at high burnup levels. The fabricated samples included pseudo-binary and higher-order compositions, allowing for the decomposition of individual fission product effects. The characterization revealed the presence of U_1-xZr_xN, Zr_1-xU_xN, ZrN, Nb_1-xU_x, U_xNb_1-x, Nb₂N, URu₃, Mo, and (U,Mo)Ru₃ as distinct fission-product-containing phases. Notably, only Zr was found to be soluble within the primary UN fuel matrix. Significant agglomeration and formation of a (Nb-rich core)–(Nb-poor shell) microstructure was observed for the Nb-containing samples. Mo was the only fission product to form metallic inclusions and the presence of Ru led to the formation of URu₃ in the pseudo-binary system (UN-10at.%Ru), or (U,Mo)Ru₃ in the higher-order samples containing 1, 1.5, and 2 at.% each of all of fission product elements i.e. UN-1at.%(ZrN, Nb, Mo, Ru). No complex nitride precipitates were found to form. The phases identified in the pseudo-binary compositions were analyzed using the Thermodynamics of Advanced Fuels-International Database (TAF-ID) and showed good agreement to experimental data, except for a possible miscibility gap in the UN-ZrN tie line and absence of the (U,Mo)Ru₃ phase.

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裂变产物在unsimfuel中的溶解度和形态

用火花等离子烧结法制备了U(X) n基SIMFUEL样品，其中X代表Zr、Nb、Mo和Ru。这些样品通过中子衍射和扫描电子显微镜进行了表征，以深入了解高燃耗水平下裂变产物的溶解度和形态。制造的样品包括伪二元和高阶成分，允许分解单个裂变产物效应。表征结果表明，U1-xZrxN、Zr1-xUxN、ZrN、Nb1-xUx、UxNb1-x、Nb2N、URu3、Mo和（U,Mo）Ru3是不同的含裂变产物相。值得注意的是，只有Zr被发现可溶于初级UN燃料基质中。在含铌样品中观察到明显的团聚和富铌核-贫铌壳微观结构的形成。Mo是唯一形成金属包裹体的裂变产物，Ru的存在导致在伪二元体系（UN-10at.%Ru）中形成URu3，或在含有1,1.5和2 at的高阶样品中形成（U,Mo）Ru3。%所有裂变产物元素，即UN-1at。%（ZrN, Nb, Mo, Ru）。未发现形成复杂的氮化物沉淀。利用先进燃料热力学-国际数据库（TAF-ID）分析了伪二元组成中的相，除了在UN-ZrN连线上可能存在混相间隙和（U,Mo）Ru3相缺失外，与实验数据吻合良好。

本文章由计算机程序翻译，如有差异，请以英文原文为准。

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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.