OXIDATION OF NUCLEAR-FUEL (UO2) BY THE PRODUCTS OF WATER RADIOLYSIS - DEVELOPMENT OF A KINETIC-MODEL
OXIDATION OF NUCLEAR-FUEL (UO2) BY THE PRODUCTS OF WATER RADIOLYSIS - DEVELOPMENT OF A KINETIC-MODEL
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DOI：
10.1016/0925-8388(94)90886-9
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发表时间：
1994-10-01
影响因子：
6.2
通讯作者：
SHOESMITH, DW
中科院分区：
文献类型：
--
作者：
CHRISTENSEN, H;SUNDER, S;SHOESMITH, DW
地下水的辐解会产生氧化剂和还原剂，这会影响放在地质处置库中的废燃料(UO2)的氧化和溶解。描述了一个描述水的辐解产物氧化UO2的动力学模型。这个模型假设UO2的单分子表面层的反应就像它被溶解在薄水中一样，其厚度与辐射分解过程中形成的自由基的扩散范围相对应。通过这种方式，我们可以使用辐解物种与溶解铀反应的速率常数，作为速率常数未知的多相体系的类似物。在一系列电化学和开路腐蚀实验的基础上，对该模型进行了改进。模型预测与在这些实验中测量的溶解速率进行了比较。
Radiolysis of groundwater will produce oxidants and reductants which can affect the oxidation and dissolution of used fuel (UO2) placed in a geological disposal vault. A kinetic model to describe the oxidation of UO2 by the products of radiolysis of water is described. This model assumes that a monomolecular surface layer of UO2 reacts as if it were dissolved in a thin layer of water of a thickness corresponding to the diffusion range of the radicals formed during radiolysis. In this manner we can use the rate constants for the reactions of radiolytic species with dissolved uranium as an analog of the heterogeneous system for which rate constants are unknown. The refinement of this model, based on a series of electrochemical and open-circuit corrosion experiments, is described. Model predictions are compared with dissolution rates measured in these experiments.