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本文在带有阴阳极的恒界面池中研究了HNO_3-N_2H_5NO_3(H_2O)/UO_2(NO_3)_2-HNO_3(30％TBP-煤油)体系中U(Ⅵ)电还原动力学。这是U(Ⅵ)电还原反萃动力学研究的第一步。测定了两相溶液中各组分浓度对U(Ⅵ)电还原速率的影响。根据实验所得数据,经回归分析得到U(Ⅵ)电还原动力学微分方程: -(d[U(Ⅵ)]/dt)=k[U(Ⅵ)]_0~(1.294)[HNO_3]_0~(0.0143)[HNO_3]_α~(0.322)[N_2H_5~+]_α~(0.0178)式中k为速度常数,25℃时,k=1.816×10~(-4)。研究了阴极电位、操作温度、两相搅拌速率和界面面积对U(Ⅵ)电还原速率的影响。选定了公称实验条件,将U(Ⅵ)电还原速率与“比”实验条件进行关联,得到如下的经验方程: r=r_0[E]~(1.589)[T]~(0.155)[W]~(0.078)[A]~(0.265)式中r_0为公称实验条件下U(Ⅵ)电还原速率。在本文实验范围内,U(Ⅵ)电还原过程由电极反应控制。
In this paper, the kinetics of U (Ⅵ) reduction in HNO_3-N_2H_5NO_3 (H_2O) / UO_2 (NO_3) _2-HNO_3 (30% TBP-kerosene) system was studied in a constant interface cell with a cathode and a cathode. This is the first step in the U (VI) electroreduction kinetic study. The effects of concentration of each component in two-phase solution on the electroreduction rate of U (Ⅵ) were measured. According to the experimental data, the kinetic differential equation of U (Ⅵ) electroreduction was obtained by regression analysis: - (d [U (Ⅵ)] / dt) = k [U (VI)] _0 ~ (1.294) [HNO3] (0.0143) [HNO_3] _α ~ (0.322) [N_2H_5 ~ +] _ α ~ (0.0178) where k is the velocity constant and k = 1.816 × 10 -4 at 25 ℃. The effects of cathodic potential, operating temperature, two-phase stirring rate and interfacial area on the electroreduction rate of U (Ⅵ) were investigated. The nominal experimental conditions were chosen to correlate the U (Ⅵ) electroreduction rate with the experimental conditions of “ratio”, and the following empirical equation was obtained: r = r_0 [E] ~ 1.589 T ~ 0.155 W [ ~ (0.078) [A] ~ (0.265) where r_0 is the electrical reduction rate of U (Ⅵ) under nominal experimental conditions. In the experimental range of this article, the U (Ⅵ) electroreduction process is controlled by the electrode reaction.