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Kinetics of oxidation and dissolution of uranium dioxide in aqueous acid solutions

机译:二氧化铀在酸水溶液中的氧化和溶解动力学

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摘要

The oxidation and dissolution of UO_2 has been studied using electrochemical methods with an UO_2 rotating disc electrode in acidic (pH 3) and non-complexing (trifluoromethanesulfonate: 0.1 mol L~(-1) NaCF_3SO_3) media. The effect of the experimental parameters such as scan rate (v) and rotation rate (ω) on the electrochemical signal has been studied. The rotation rate of the electrode does not influence the resulting signal, which indicates that only a charge transfer is involved in the UO_2 oxidation kinetic. However, scan rate variations show different reactions involved in the UO_2 oxidation. Linear sweep voltammetry and cyclic voltammetry coupled to X-ray photoelectron spectroscopy (XPS) and inductively coupled plasma mass spectrometry (ICP-MS) measurements suggest two successive electrochemical reactions with an exchange of one electron for each of them and the formation of one intermediate species of U(V).
机译:使用电化学方法,在酸性(pH 3)和非络合(三氟甲磺酸盐:0.1 mol L〜(-1)NaCF_3SO_3)介质中,采用UO_2旋转盘电极对UO_2的氧化和溶解进行了研究。研究了诸如扫描速率(v)和旋转速率(ω)等实验参数对电化学信号的影响。电极的旋转速率不影响所得信号,这表明在UO_2氧化动力学中仅涉及电荷转移。然而,扫描速率的变化表明UO_2氧化涉及不同的反应。线性扫描伏安法和循环伏安法与X射线光电子能谱(XPS)耦合和电感耦合等离子体质谱(ICP-MS)测量表明,两个连续的电化学反应中每个交换一个电子,并形成一个中间物种的U(V)。

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