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首页> 外文期刊>The journal of physical chemistry, C. Nanomaterials and interfaces >Radiolytic Corrosion of Uranium Dioxide: Role of Molecular Species
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Radiolytic Corrosion of Uranium Dioxide: Role of Molecular Species

机译:二氧化铀的放射性腐蚀:分子种类的作用

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In this work, the oxidative corrosion of UO2 particles by molecular species produced by ~4He~(2+) radiolysis of water (simulated by irradiation with a ~4He~(2+) beam) has been investigated as a function of the absorbed dose under open and closed atmospheres. This work was carried out by coupling for the first time (1) characterization of the UO2 surface after oxidation, (2) analysis of H2 and H2O2 produced by water radiolysis, and (3) quantification of the uranium species leached into the solution during irradiation. Oxidation of the surface of the UO2 particles was characterized by Raman spectroscopy. H2 and H2O2 were analyzed by micro gas chromatography and UV-vis spectrophotometry, respectively. Inductively coupled plasma mass spectrometry was used to quantify the soluble uranium species released into the solution. The results showed that, when the ultrapure water above the UO2 particles was irradiated in an open atmosphere, metastudtite was formed on the UO2 surface, indicating its oxidation by the H2O2 produced by water radiolysis. This oxidation was accompanied by migration of soluble uranium species [U(VI)] into the irradiated solution. After irradiation in a closed atmosphere, oxidation of the UO2 surface and migration of soluble uranium species were limited due to the presence of H2. The inhibition does not occur by direct effect of H2 on H2O2 but more probably by adsorption of H2 molecules on the UO2 surface.
机译:在这项工作中,研究了UO2颗粒被水〜4He〜(2+)放射分解产生的分子种类(通过〜4He〜(2+)束辐照模拟)产生的氧化腐蚀与吸收剂量的函数关系。在开放和封闭的气氛下。这项工作是通过以下方式首次进行的:(1)氧化后表征UO2表面;(2)分析由水分解产生的H2和H2O2;(3)量化照射过程中浸出到溶液中的铀物种。通过拉曼光谱法表征UO 2颗粒的表面氧化。 H2和H2O2分别通过微型气相色谱和紫外可见分光光度法进行分析。电感耦合等离子体质谱法用于量化释放到溶液中的可溶性铀物质。结果表明,当在敞开的气氛中照射UO2颗粒上方的超纯水时,在UO2表面形成偏硅酸盐,表明其被水分解产生的H2O2氧化。这种氧化伴随着可溶铀物质[U(VI)]迁移到辐照溶液中。在封闭的气氛中照射后,由于存在H2,UO2表面的氧化和可溶性铀物质的迁移受到限制。抑制作用不是通过H2对H2O2的直接作用而发生的,而可能是通过H2分子在UO2表面的吸附而发生的。

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