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有机还原剂作为一类无盐试剂被广泛研究,其可应用于Purex流程的改进。本工作研究氨基羟基脲与Pu(Ⅳ)的还原反应动力学。实验测得还原反应动力学方程为:-dc(Pu(Ⅳ))/dt=kc(Pu(Ⅳ))c1.06(HSC)c-0.43(H+)c-0.58(NO3-)。其中,在22.1℃时,k=(11.8±1.1)(mol/L)-0.05·s-1,活化能Ea=(70.96±1.0)kJ/mol。实验研究了氨基羟基脲浓度、H+浓度、NO3-浓度、Fe3+浓度、UO22+浓度对该还原反应速率的影响。提高氨基羟基脲浓度、降低H+浓度和NO3-浓度、Pu(Ⅳ)的还原速度加快;UO22+浓度和Fe3+浓度对Pu(Ⅳ)的还原速度基本无影响。
Organic reductants have been extensively studied as a class of salt-free reagents that can be applied to Purex process improvements. This work is to study the kinetics of reduction of aminohydroxyurea and Pu (Ⅳ). The kinetics of the reduction reaction was measured as follows: -dc (Pu (Ⅳ)) / dt = kc (Pu (Ⅳ)) c1.06 (HSC) c-0.43 (H +) c-0.58 (NO3-). Among them, k = (11.8 ± 1.1) (mol / L) -0.05 · s-1 and activation energy Ea = (70.96 ± 1.0) kJ / mol at 22.1 ℃. The effects of amino hydroxy urea concentration, H + concentration, NO3- concentration, Fe3 + concentration and UO22 + concentration on the reduction reaction rate were studied experimentally. Increasing the concentration of aminohydroxyurea and decreasing the concentrations of H + and NO3- accelerated the reduction of Pu (Ⅳ). The reduction of Pu (Ⅳ) did not affect the reduction rate of Pu (Ⅳ) at concentrations of UO22 + and Fe3 +.