Gd2O3 Doped UO2(s) Corrosion in the Presence of Silicate and Calcium under Alkaline Conditions

IF 3.1 4区化学 Q2 CHEMISTRY, INORGANIC & NUCLEAR

Inorganics Pub Date : 2023-12-01 DOI:10.3390/inorganics11120469

Sonia García-Gómez, J. Giménez, I. Casas, Jordi Llorca, Joan De Pablo

引用次数: 0

Abstract

The anodic reactivity of UO2 and UO2 doped with Gd2O3 was investigated by electrochemical methods in slightly alkaline conditions in the presence of silicate and calcium. At the end of the experiments, the electrodes were analysed by X-ray photoelectron spectroscopy to determine the oxidation state of the uranium on the surface. The experiments showed that the increase in gadolinia doping level led to a reduction in the reactivity of UO2, this effect being more marked at the highest doping level studied (10 wt.% Gd2O3). This behaviour could be attributed to the formation of dopant-vacancy clusters (GdIII-Ov), which could limit the accommodation of excess O2− into the UO2 lattice. In addition, the presence of Ca2+ and SiO32− decreased the anodic dissolution of UO2. In summary, the Gd2O3 doping in presence of silicate and calcium was found to strongly decrease the oxidative dissolution of UO2, which is a beneficial situation regarding the long-term management of spent nuclear fuel in a repository.

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碱性条件下硅酸盐和钙存在时掺杂 Gd2O3 的氧化铀（s）的腐蚀作用

采用电化学方法研究了微碱性条件下硅酸钙存在下UO2和掺杂Gd2O3的UO2的阳极反应性。在实验结束时，用x射线光电子能谱分析电极，以确定表面铀的氧化状态。实验表明，钆掺杂量的增加导致UO2反应性的降低，这种影响在研究的最高掺杂量(10 wt.% Gd2O3)时更为明显。这种行为可以归因于掺杂空位团簇(GdIII-Ov)的形成，这可以限制过量的O2−进入UO2晶格。此外，Ca2+和SiO32−的存在降低了UO2的阳极溶解。综上所述，在硅酸盐和钙的存在下，Gd2O3掺杂可以显著降低UO2的氧化溶解，这对于乏燃料在储存库中的长期管理是有利的。

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

Inorganics Chemistry-Inorganic Chemistry

CiteScore

2.80

自引率

10.30%

发文量

193

审稿时长

6 weeks

期刊介绍： Inorganics is an open access journal that covers all aspects of inorganic chemistry research. Topics include but are not limited to: synthesis and characterization of inorganic compounds, complexes and materials structure and bonding in inorganic molecular and solid state compounds spectroscopic, magnetic, physical and chemical properties of inorganic compounds chemical reactivity, physical properties and applications of inorganic compounds and materials mechanisms of inorganic reactions organometallic compounds inorganic cluster chemistry heterogenous and homogeneous catalytic reactions promoted by inorganic compounds thermodynamics and kinetics of significant new and known inorganic compounds supramolecular systems and coordination polymers bio-inorganic chemistry and applications of inorganic compounds in biological systems and medicine environmental and sustainable energy applications of inorganic compounds and materials MD