Exploring cluster formation in uranium oxidation using high resolution X-ray spectroscopy at elevated temperatures.

IF 7.5 Q1 MATERIALS SCIENCE, MULTIDISCIPLINARY
Communications Materials Pub Date : 2025-01-01 Epub Date: 2025-04-17 DOI:10.1038/s43246-025-00795-2
Elena F Bazarkina, Stephen Bauters, Yves Watier, Stephan Weiss, Sergei M Butorin, Kristina O Kvashnina
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引用次数: 0

Abstract

Uranium dioxide (UO2) is a complex material with significant relevance to nuclear energy, materials science, and fundamental research. Understanding its high-temperature behavior is crucial for developing new uranium-based materials and improving nuclear fuel efficiency in nuclear reactors. Here we study the evolution of uranium state during the oxidation of UO2 in air at temperatures up to 550 °C using the in situ X-ray absorption spectroscopy in high energy resolution fluorescence detection mode at the U M4 edge, combined with electronic structure calculations. Our data reveal a complex sequence of events occurring over minutes and hours at elevated temperatures, including changes in the electronic and local structure, 5 f electron occupancy, the formation of U cuboctahedral clusters, and the creation of U4O9 and U3O7 mixed U oxide phases. These findings highlight the fundamental role of clustering processes and pentavalent uranium in both the oxidation process and the stabilization of uranium materials.

利用高分辨率x射线光谱在高温下探索铀氧化中的团簇形成。
二氧化铀(UO2)是一种复杂的材料,与核能、材料科学和基础研究有着重要的关系。了解其高温行为对于开发新的铀基材料和提高核反应堆的核燃料效率至关重要。本文利用高能分辨率荧光检测模式下的原位x射线吸收光谱技术,结合电子结构计算,研究了在高达550℃的温度下UO2在空气中氧化过程中铀态的演变。我们的数据揭示了在高温下发生的一系列复杂事件,包括电子和局部结构的变化,5f电子占用,U立方体簇的形成,以及U4O9和U3O7混合U氧化物相的形成。这些发现突出了聚类过程和五价铀在铀材料氧化过程和稳定化中的基本作用。
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
Communications Materials
Communications Materials MATERIALS SCIENCE, MULTIDISCIPLINARY-
CiteScore
12.10
自引率
1.30%
发文量
85
审稿时长
17 weeks
期刊介绍: Communications Materials, a selective open access journal within Nature Portfolio, is dedicated to publishing top-tier research, reviews, and commentary across all facets of materials science. The journal showcases significant advancements in specialized research areas, encompassing both fundamental and applied studies. Serving as an open access option for materials sciences, Communications Materials applies less stringent criteria for impact and significance compared to Nature-branded journals, including Nature Communications.
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