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Recalculation of oxygen isotope fractionation of uranium trioxide

机译:重新计算三氧化铀的氧同位素分馏

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摘要

Uranium is an element with a large radius and atomic mass, so its oxides are considered to be of very low δ~(18)O value at the bottom of the ~(18)O enrichment table for minerals. The oxygen isotope fractionation between uranium dioxide, uranium trioxide and water has been calculated by Hattori & Halas using force constants and low temperature heat capacity, which is a rare example for spectrum-heat capacity model (SHCM). But one could find some problems after detailed analysis of the calculated results. The force constants of uranium oxides are listed in table 1. Compared with the force constants of UO_2, K_2 of α-UO_3 is approximately equal to K_1 and F of α-UO_3 is obviously larger than that of UO_2. But α-UO_3 are depleted in ~(18)O comparedwith UO_2 in the calculation of Hattori & Halas. As we know, bonds with large force constants and small atomic mass will produce high vibrational frequencies and tend to be incorporated by heavy isotopes, which makes us feel hard to understand the calculation results of Hattori & Halas. For this reason, the oxygen isotope fractionation of α-UO_3 is recalculated using the spectroscopic data of Tsuboi and the modified increment method of Zheng.
机译:铀是一种具有大半径和原子量的元素,因此铀的氧化物在矿物〜(18)O富集表底部的δ〜(18)O值非常低。 Hattori&Halas使用力常数和低温热容计算出了二氧化铀,三氧化铀和水之间的氧同位素分馏,这在光谱热容模型(SHCM)中是一个罕见的例子。但是,对计算结果进行详细分析后,可能会发现一些问题。铀氧化物的力常数列于表1。与UO_2的力常数相比,α-UO_3的K_2近似等于K_1,α-UO_3的F明显大于UO_2。在Hattori&Halas的计算中,与UO_2相比,α-UO_3的〜(18)O减少了。众所周知,具有大的力常数和较小的原子量的键会产生较高的振动频率,并倾向于被重同位素所吸收,这使我们很难理解Hattori&Halas的计算结果。因此,使用Tsuboi的光谱数据和Zheng的修正增量法重新计算α-UO_3的氧同位素分馏。

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