Multi-scale structural investigation of hypo-stoichiometric (U1-yPuy)O1.98 oxides with high plutonium content

IF 5.8 2区材料科学 Q1 MATERIALS SCIENCE, CERAMICS

Journal of The European Ceramic Society Pub Date : 2025-06-13 DOI:10.1016/j.jeurceramsoc.2025.117623

M.-M. Desagulier , J. Martinez , P.M. Martin , F. Lebreton , M.O.J.Y. Hunault , C. Guéneau , N. Clavier

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Abstract

A significant lack of experimental data concerning the thermophysical properties of U_1-yPu_yO_2-x for high Pu contents (y > 0.45) is observed. To bridge this gap, dense, monophasic, stoichiometric and homogenous oxides U_1-yPu_yO_2.00 samples (with y = 0.60–0.70) were initially manufactured and characterized. To study the impact of the Oxygen/Metal ratio on thermal properties, hypo-stoichiometric samples were obtained from the previous batches. The strategy was to optimize annealing to reach O/M = 1.98 and perform multi-scale characterizations (optical microscopy, X-ray diffraction, Raman spectroscopy, electron probe microanalysis and X-ray Absorption Near Edge Structure). These revealed monophasic and hypo-stoichiometric samples with a homogeneous chemical distribution of cations and oxygen and a complex redox cations speciation: U(IV)/U(V), Pu(III)/Pu(IV) and Am(III). The results demonstrate the potential of these samples for measuring thermophysical properties, and enable the extension of the Pu content validation range of some empirical laws from y = 0.45–0.69.

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高钚含量低化学计量（u1ypuy）O1.98氧化物的多尺度结构研究

对于高Pu含量（y >； 0.45），U1-yPuyO2-x的热物理性质明显缺乏实验数据。为了弥补这一差距，最初制造了致密的、单相的、化学计量的和均相的氧化物U1-yPuyO2.00样品（y = 0.60-0.70）并对其进行了表征。为了研究氧/金属比对热性能的影响，从前几批样品中获得了低化学计量样品。策略是优化退火达到O/M = 1.98，并进行多尺度表征（光学显微镜，x射线衍射，拉曼光谱，电子探针微分析和x射线吸收近边结构）。这些结果揭示了单相和低化学计量样品具有均匀的阳离子和氧的化学分布和复杂的氧化还原阳离子形态：U(IV)/U(V), Pu(III)/Pu（IV）和Am（III）。结果表明，这些样品具有测量热物性的潜力，并能够将一些经验定律的验证范围从y = 0.45-0.69扩展。

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来源期刊

Journal of The European Ceramic Society 工程技术-材料科学：硅酸盐

CiteScore

10.70

自引率

12.30%

发文量

863

审稿时长

35 days

期刊介绍： The Journal of the European Ceramic Society publishes the results of original research and reviews relating to ceramic materials. Papers of either an experimental or theoretical character will be welcomed on a fully international basis. The emphasis is on novel generic science concerning the relationships between processing, microstructure and properties of polycrystalline ceramics consolidated at high temperature. Papers may relate to any of the conventional categories of ceramic: structural, functional, traditional or composite. The central objective is to sustain a high standard of research quality by means of appropriate reviewing procedures.