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由1BP料液制备2AF料液的过程中需要氧化去除1BP中还原剂,同时将Pu(Ⅲ)氧化至Pu(Ⅳ)。以气液并流模式在玻璃填料柱中研究了亚硝气对模拟1BP料液中还原剂的氧化情形,考察了亚硝气用量、料液停留时间、HNO_3浓度和温度对模拟1BP料液中还原剂氧化率的影响。结果表明:25℃时,在羟胺、肼浓度均约为0.08mol/L,c(HNO_3)=1.5mol/L、ρ_0(U(Ⅳ))=1.26g/L、Pu(Ⅲ)(以Fe(Ⅱ)代替)质量浓度为8.76g/L的1BP料液中,当N_2O_4液体为还原剂总量的1.2倍(摩尔比)、停留时间为3min时,1BP料液中还原剂的氧化率达到99.9%以上,Pu(Ⅲ)的氧化率在99.9%以上。
The preparation of 2AF from 1BP feedstock requires oxidation to remove reductant from 1BP while Pu (Ⅲ) is oxidized to Pu (Ⅳ). The gas-liquid cocurrent mode was used to study the oxidation of reductant by nitrous gas in simulated 1BP feedstock in a glass packed column. The effects of nitrous oxide consumption, feedstock residence time, HNO_3 concentration and temperature on the performance of simulated 1BP feedstock Effect of reductant oxidation rate. The results showed that the concentrations of hydroxylamine and hydrazine were about 0.08mol / L, c (HNO3) = 1.5mol / L, ρ_0 (U (Ⅳ)) = 1.26g / L at 25 ℃. (Ⅱ) instead of 1, the rate of oxidation of the reductant in 1BP feed liquid was reached when the concentration of N_2O_4 liquid was 1.2 times (molar ratio) of the total amount of reductant and the residence time was 3min in 1BP feed solution with mass concentration of 8.76g / L 99.9%, Pu (Ⅲ) oxidation rate of 99.9% or more.