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氧化铈（III）与二氧化铀的共沉淀

Coprecipitation of Ce(III) oxide with UO.

作者信息

Saleh M, Hedberg M, Tam P L, Spahiu K, Persson I, Ekberg C

机构信息

Nuclear Chemistry / Industrial Materials Recycling, Chalmers University of Technology, SE-412 96 Gothenburg, Sweden.

Department of Industrial and Materials Science, Chalmers University of Technology, SE-412 96 Gothenburg, Sweden.

出版信息

J Synchrotron Radiat. 2024 Nov 1;31(Pt 6):1489-1504. doi: 10.1107/S1600577524008336. Epub 2024 Sep 30.

DOI:10.1107/S1600577524008336
PMID:39347702
原文链接:https://pmc.ncbi.nlm.nih.gov/articles/PMC11542660/
Abstract

The neutralization of acidic solutions containing U (IV) and Ce (III) at room temperature in glove box atmosphere and in the presence of dithionite results in coprecipitation of these elements as amorphous solid solutions CeUO. The solubilities of the precipitates with different mole fractions (x) of Ce(OH) (x = 0.01 or 0.1) were determined in 1 M NaClO solutions between pH 2.2 and 12.8 under reducing conditions. The solids were investigated by a variety of methods (chemical analysis, SEM-EDX, XRD, XPS, XAS) to determine the nature of the solid solutions formed, their composition and the valence state of Ce and U. X-ray photoelectron spectroscopy confirmed the oxidation states of the solids both before and after the equilibration as Ce (III) and U (IV). The amorphous coprecipitates reached equilibrium relatively fast (∼1 week). The release of Ce from the coprecipitates was totally dominated by the release of uranium over the whole pH range. The Ce concentrations decrease slightly with the decrease of Ce content in the solid, suggesting that CeUO solids behave thermodynamically as solid solutions. The concentrations of U in equilibrium with the coprecipitate were in excellent agreement with the solubility of UO(s) under reducing conditions reported in the literature. The conditional solubility product of Ce(OH) from the coprecipitate was several orders of magnitude (∼4 in the near neutral pH range and ∼18 in the acidic range) lower than that of pure Ce(OH)(s). The activities and activity coefficients of Ce(OH)(s) in the coprecipitate were also estimated. Activity coefficients are much less than 1, indicating that the mixing of Ce(OH) with UO is highly favorable.

摘要

在手套箱气氛中于室温下，在连二亚硫酸盐存在的情况下，对含有U(IV)和Ce(III)的酸性溶液进行中和，会使这些元素以非晶态固溶体CeUO的形式共沉淀。在还原条件下，测定了在pH值为2.2至12.8的1 M NaClO溶液中，不同摩尔分数（x）的Ce(OH)（x = 0.01或0.1）沉淀物的溶解度。通过多种方法（化学分析、扫描电子显微镜-能谱仪、X射线衍射、X射线光电子能谱、X射线吸收光谱）对固体进行研究，以确定形成的固溶体的性质、其组成以及Ce和U的价态。X射线光电子能谱证实了平衡前后固体的氧化态均为Ce(III)和U(IV)。非晶态共沉淀物相对较快地达到平衡（约1周）。在整个pH范围内，共沉淀物中Ce的释放完全由铀的释放主导。Ce浓度随着固体中Ce含量的降低而略有下降，这表明CeUO固体在热力学上表现为固溶体。与共沉淀物平衡的U浓度与文献报道的还原条件下UO(s)的溶解度非常吻合。共沉淀物中Ce(OH)的条件溶度积比纯Ce(OH)(s)的溶度积低几个数量级（在近中性pH范围内约为4，在酸性范围内约为18）。还估算了共沉淀物中Ce(OH)(s)的活度和活度系数。活度系数远小于1，表明Ce(OH)与UO的混合非常有利。

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