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Vaporization chemistry of hypo-stoichiometric (U,Pu)O-2

机译:低化学计量(U,Pu)O-2的汽化化学

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Calculations were performed on hypo-stoichiometric uranium plutonium di-oxide to examine its vaporization behavior as a function of O/M (M = U + Pu) ratio and plutonium content. The phase U(1-y)PuyOz was treated as an ideal solid solution of (1-y)UO2+yPuO((2-x)) such that x=(2-z)/y. Oxygen potentials for different desired values of y,z, and temperature were used as the primary input to calculate the corresponding partial pressures of various O-, U-, and Pu-bearing gaseous species. Relevant thermodynamic data for the solid phases UO2 and PuO(2-x) and the gaseous species were taken from the literature. Total vapor pressure varies with O/M and goes through a minimum. This minimum does not indicate a congruently vaporizing composition. Vaporization behavior of this system can at best be quasi-congruent. Two quasi-congruently vaporizing compositions (QCVCs) exist, representing the equalities (O/M)(vapor)=(O/M)(mixed-oxide) and (U/Pu)(vapor)=(U/Pu)(mixed-oxide), respectively. The (O/M) corresponding to QCVC1 is lower than that corresponding to QCVC2, but very close to the value where vapor pressure minimum occurs. The O/M values of both QCVCs increase with decrease in plutonium content. The vaporization chemistry of this system, on continuous vaporization under dynamic condition, is discussed. (C) 2001 Elsevier Science B.V. All rights reserved. [References: 12]
机译:对化学计量比低的铀二氧化performed进行了计算,以检查其气化行为随O / M(M = U + Pu)比和p含量的变化。将相U(1-y)PuyOz视为(1-y)UO2 + yPuO((2-x))的理想固溶体,以使x =(2-z)/ y。 y,z和温度的不同期望值的氧气电势用作主要输入,以计算各种O,U和Pu气态物质的相应分压。固相UO2和PuO(2-x)以及气态物质的相关热力学数据均来自文献。总蒸气压随O / M的变化而变化,并达到最小值。该最小值不表示完全蒸发的组合物。该系统的汽化行为最多可以是完全一致的。存在两种准全气化成分(QCVC),分别表示等式(O / M)(蒸气)=(O / M)(混合氧化物)和(U / Pu)(蒸气)=(U / Pu)(混合) -氧化物)。对应于QCVC1的(O / M)低于对应于QCVC2的(O / M),但非常接近发生蒸气压最小值的值。两个QCVC的O / M值都随着p含量的减少而增加。讨论了该系统在动态条件下连续汽化的汽化化学性质。 (C)2001 Elsevier Science B.V.保留所有权利。 [参考:12]

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