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作 者:常利[1] 张倩[1] 郭建华[1] 刘利生[1] 王长水[1] 常尚文[1] 李瑞雪[1] 欧阳应根[1] 田保生[1]
机构地区:[1]中国原子能科学研究院放射化学研究所,北京102413
出 处:《核化学与放射化学》2012年第4期218-222,共5页Journal of Nuclear and Radiochemistry
摘 要:为了避免引入过多试剂,针对后处理Purex流程中将Pu(Ⅲ)氧化到Pu(Ⅳ)的调价过程,研究了一种新的催化氧化工艺。研究了在不同温度、酸度、肼浓度等条件下,硝酸体系中Pu(Ⅲ)的Pt催化氧化行为。结果表明:硝酸介质中Pu(Ⅲ)可以被Pt催化氧化为四价;在70℃条件下,当硝酸浓度大于3mol/L时,含支持还原剂肼的溶液中Pu(Ⅲ)的催化氧化调价可以很快实现,Pu(Ⅲ)氧化率大于99.9%;提高温度、加大酸度均有利于Pu(Ⅲ)的氧化;支持还原剂肼的量对其的催化氧化有一定的影响,肼的浓度升高,催化氧化的诱导期变长。In order to avoid introducing non-combustible reagents during the valence adjust- ments of Pu in the Purex process for nuclear fuel reprocessing, a new catalytic oxidation technology for conversion of Pu( Ⅲ ) to Pu(Ⅳ) was studied in this paper. The influence of temperature, nitric acid concentration, and hydrazine concentration on the completeness and kinetics of Pt-catalyzed oxidation of Pu( Ⅲ ) was investigated. The experimental results show that in the presence of a platinum gauze catalyst Pu( Ⅲ ) in a hydrazine-containing solution can be quickly and almost quantitatively (〉99.9%) oxidized to Pu(Ⅳ) at 70℃ and nitric acid concentrations higher than 3 mol/L. The increase of HNO3 concentration and elevation of temperature favores the oxidation of Pu( Ⅲ ). The concentration of hydrazine also shows some influence: the higher the concentration of hydrazine is, the longer the induction period will be.
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