Pu(Ⅲ)光氧化工艺研究
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摘要: 对Purex工艺流程中IBP和2BP混合液流进行了紫外光照射,实现了Pu(Ⅲ)光氧化至Pu(Ⅳ)的“无盐”调价过程。光照7.5h可使Pu(Ⅲ)全部氧化成Pu(Ⅳ),Pu(Ⅵ)含量<1%,继续光照2.5h仍能控制Pu(Ⅵ)含量<7%。研究了Pu、HNO_3、Fe ̄(2+)浓度以及光源功率、温度变化对Pu(Ⅲ)光氧化的影响。结果表明:在Fe ̄(2+)和浓度基本维持恒定的情况下,Pu从0.30g/1、0.66g/1增至1.14g/1,HNO_3从1.5mol/l增至2.7mol/l,对Pu(Ⅲ)光氧化基本无影响;在相同条件下,光源功率增大,温度升高,Pu(Ⅲ)光氧化时间减少。此外,还对光照后溶液中Pu价态稳定性与放置时间的关系,进行了5次10天的跟踪测定。结果表明,Pu的价态在10天内基本稳定。Abstract: STUDY ON PHOTOOXIDATION OF PLUT0NIUM(Ⅲ)0F 1BP IN PUREX PROCESSZHOU ZHIHONG; HU JINGXIN; DUAN YUNFU; ZHANG XIANYE(China Institutei of atomic Energy,P. O. Box 275(26),BEIJING 102413)XIE XUEYI; JIA RUIHE; WANG SHUIXIANG(Lanzhou Nuclear Fuel Complex,Lanzhou 732850)ABSTRACT Bench scale of photcooxidation plutonium(Ⅲ)of 1BP to plutonium(Ⅳ)in Purex processinstead of adding sedium nitrite has been achieved by UV Iight irradiation. The alternative tech-nology can realize so-called solt-free process. The about 99%of plutonium(Ⅲ) is oxidized to plu-tonium(Ⅳ) at 7.5h,but plutonium(Ⅵ)is less than 1%,extending 2.5h of irradiation,less than7%plutonium(Ⅵ)can be controled.The effects of concentration of plutonium ,nitric acid andferrous ion and of power of light source and of temperature on photooxidation of plutonium(Ⅲ)have been investegated.The results show that,in the constant conditions of concentration of fer-rous ion and hydrazine,changing concentration of plutonium from 0.30,0.66 to 1.14g/1,concen-tration of nitric acid from 1.5 to 2.7 mol/l,the photcoxidation of plutonium(Ⅲ) is not effected.In the same conditions,the time of photcoxidation of plutonium(Ⅲ)decreases with the increaseof power of light source and with increase of temperature. In addition,the effects of keeping timeof solution irradiated on the change of valence of plutonium have been observed. The results showthat the valence of plutonium dose not change in ten days.Key words Photcoxidation Pu(Ⅲ)Purex process Salt-free process