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Thermochemical modeling of the U_(1-y)Gd_yO_(2±x) phase

机译:U_(1-Y)GD_YO_(2±x)阶段的热化学建模

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Urania (UO2) has the remarkable characteristic of exhibiting oxygen nonstoichiometry while maintaining the flourite crystal structure through oxygen vacancy formation and additions of oxygen atoms to interstitial anion sublattice sites. The convention is to denote the phase as UO_(2±x); the oxygen potential in equilibrium with UO_(2±x) determines the value of x. Characterizing the equilibrium oxygen partial pressure of urania at specific temperatures and oxygen to metal ratios (O/M) is a useful way to understand the thermochemistry and stability of the phase. The deviation from oxygen stoichiometry of urania is affected by additives or fission products that dissolve in the fluorite solid solution. Yttrium and many lanthanides (Ln), such as Ce and La, are high yield fission products or longer lived daughters of fission products and are readily dissolved in the fluorite matrix. Gadolinium is not a high yield fission or activation product; however, it can be added as a burnable poison and is soluble in urania. Gd can be present up to 10 percent by weight in fresh UO2 fuel; therefore, understanding the thermochemistry of the U_(1-y)Gd_yO_(2±x) solid solution is important for development of a comprehensive and self-consistent thermodynamic database to describe phase equilibria in oxide nuclear fuels. The objective of the effort reported here is a Gibbs energy model of the fluorite phase U_(1-y)Gd_yO_(2±x) using a three sublattice compound energy formalism (CEF) representation. The CEF for U_(1-y)Gd_yO_(2±x) can be readily integrated into more complex multicomponent models of the UO2 fluorite phase within a database framework; indeed, the model presented in this work is an extension of the one developed for UO_(2±x) by Gueneau et al.
机译:乌兰尼亚(UO2)具有在将氟晶体结构通过氧空位形成和添加氧原子的同时表现出氧气非沸石的显着特征,并在间质Hythial Anion Sublattice位点保持。 “公约”是表示阶段作为UO_(2±x);含有UO_(2±x)的氧气电位确定x的值。特征在特定温度和氧气对金属比(O / M)的urania的平衡氧分压是理解阶段热化学和稳定性的有用方法。从乌兰尼亚的氧化学计量偏差受溶解在萤石固溶体中的添加剂或裂变产物的影响。 YTTRIUM和许多镧系元素(LN),例如CE和LA,是高产裂变产品或较长的裂变产物的寿命,并且易于溶解在萤石基质中。钆不是高产裂变或活化产品;然而,它可以作为可燃的毒药添加,可溶于乌兰尼亚。 Gd在新鲜UO2燃料中可以呈现高达10%的重量;因此,了解U_(1-Y)GD_YO_(2±X)固体解决方案的热化学,对于开发综合和自我一致的热力学数据库来说是重要的,以描述氧化物核燃料中的相平衡。这里报道的努力的目的是使用三个子分子化合物能量形式(CEF)表示的萤石相U_(1-Y)Gd_yo_(2±x)的Gibbs能量模型。 U_(1-Y)GD_YO_(2±x)的CEF可以容易地集成到数据库框架内更复杂的UO2萤石相的多组分模型;实际上,在这项工作中提供的模型是由Guenau等人为UO_(2±x)开发的模型。

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