溶剂萃取法从辐照镎靶中提取分离~(238)Pu(Ⅰ):镎钚共去污循环
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- 英文论文题名：Separation of ~(238)Pu from irridated Np target by solvent extraction(Ⅰ):Np and Pu co-decontamination cycle
- 论文作者：蒋德祥 ; 何辉 ; 周贤明 ; 陈延鑫 ; 刘金平 ; 叶国安 ; 唐洪彬
- 英文论文作者：JIANG De-xiang ; HE Hui ; ZHOU Xian-ming ; CHEN Yan-xing ; LIU Jin-ping ; YE Guo-an ; TANG Hong-bin ; China Institute of Atomic Energy
- 年：2015
- 作者机构：中国原子能科学研究院,放射化学研究所;
- 论文关键词：钚-238 ; 辐照镎靶 ; 溶剂萃取 ; 偏二甲基肼
- 英文论文关键词：Pu-238 ; irridated Np target ; solvent extraction ; 1'1-dimethyl hydrazine
- 会议召开时间：2015-09-21
- 会议录名称：中国核科学技术进展报告（第四卷）——中国核学会2015年学术年会论文集第6册（核化学与放射化学分卷、核化工分卷）
- 语种：中文
- 分类号：TL241
- 学会代码：EGVD
- 会议名称：中国核学会2015年学术年会
- 会议地点：中国四川绵阳
- 主办单位：中国核学会
- 学会名称：中国核学会
- 页数：9
- 文件大小：383k
- 原文格式：O
- 会议级别：全国
摘要
考察了80℃条件下偏二甲基肼(UDMH)还原Np(Ⅴ),Pu(Ⅳ)的反应,结果表明镎钚能以较快的速度还原为Np(Ⅳ)和Pu(Ⅲ);获得了UDMH与HNO_2发生反应的计量比为1:1;并得到了HNO_2将UDMH-Np(Ⅳ)-Pu(Ⅲ)体系中钚氧化为Pu(Ⅳ)、镎保持为Np(Ⅳ)的条件。在此基础上,设计并验证了以TBP为萃取剂从辐照镎靶溶解液中分离提取~(238)Pu的镎钚共去污循环工艺。该工艺分为镎-钚共萃取、钚反萃、镎反萃三个部分。串级实验的验证结果表明,在镎钚共萃取工艺段,采用偏二甲基肼(UDMH)还原-亚硝酸氧化两步法可将镎钚同时保持为Np(Ⅳ)与Pu(Ⅳ),选用20%TBP/煤油萃取体系,可实现镎与钚的萃取率均在99.5%以上,可实现镎钚共萃取;在钚反萃工艺段,选用氨基磺酸亚铁为还原剂并保持补萃段HNO_3浓度7 mol/L,钚的反萃率达到99.97%,镎的反萃率仅为0.81%,可实现镎钚分离;在镎反萃工艺段,镎反萃率在99.5%以上,可将镎反萃进入水相。
The reduction of Np(Ⅴ) and Pu(Ⅳ) by 1'1-dimethyl hydrazine(UDMH) at 80 ℃ were studied,the result showed that neptunium and plutonium could be reduced to Np(Ⅳ) and Pu(Ⅲ)quickly with a stoichiometry as 1:1 between UDMH and HNO_2.The operation of oxidizing neptunium and plutonium in the solution containing UDMH-Np(Ⅳ)-Pu(Ⅲ) to Np(Ⅳ) and Pu(Ⅳ)by HNO_2 was examitated.Based on these studies,the extraction of ~(238)Pu from the dissolution solution of irridated neptunium target was designed and validated.Such an extraction includes three units,the co-extraction of plutonium and neptunium,the stripping of Pu and the stripping of Np.The results of cascade experiments showed that in the co-extraction of Np and Pu stage,Np and Pu could be maintained in Np(Ⅳ) and Pu(Ⅳ) simultaneously using UDMH reduction and HNO_2 oxidation two-step method.The extraction ratio of Np and Pu can be obtained above 99.5% by the 20%TBP/OK extraction system.In the plutonium stripping unit,the stripping of Pu reaches 99.97% and stripping ratio of Np was only 0.81% with Fe(NH_2SO_3)_2 as the stripping agent and maintaining the nitric acid concentration in complementary extraction unit up to 7 mol/L.In the neptunium stripping stage,the neptunium stripping ratio was higher than 99.5%.
The reduction of Np(Ⅴ) and Pu(Ⅳ) by 1'1-dimethyl hydrazine(UDMH) at 80 ℃ were studied,the result showed that neptunium and plutonium could be reduced to Np(Ⅳ) and Pu(Ⅲ)quickly with a stoichiometry as 1:1 between UDMH and HNO_2.The operation of oxidizing neptunium and plutonium in the solution containing UDMH-Np(Ⅳ)-Pu(Ⅲ) to Np(Ⅳ) and Pu(Ⅳ)by HNO_2 was examitated.Based on these studies,the extraction of ~(238)Pu from the dissolution solution of irridated neptunium target was designed and validated.Such an extraction includes three units,the co-extraction of plutonium and neptunium,the stripping of Pu and the stripping of Np.The results of cascade experiments showed that in the co-extraction of Np and Pu stage,Np and Pu could be maintained in Np(Ⅳ) and Pu(Ⅳ) simultaneously using UDMH reduction and HNO_2 oxidation two-step method.The extraction ratio of Np and Pu can be obtained above 99.5% by the 20%TBP/OK extraction system.In the plutonium stripping unit,the stripping of Pu reaches 99.97% and stripping ratio of Np was only 0.81% with Fe(NH_2SO_3)_2 as the stripping agent and maintaining the nitric acid concentration in complementary extraction unit up to 7 mol/L.In the neptunium stripping stage,the neptunium stripping ratio was higher than 99.5%.
引文
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[15]A.A.柴霍尔斯基,邱孝熹译,林漳基校,镎化学[M].北京:原子能出版社,1986.
[16]李小该.APOR流程1B槽中镎的走向行为研究[D].北京:中国原子能科学研究院,2009.
[2]R.W.Mckee,D.E.Deonigi,D.R.Haffner Isotope Productions For U.S.Nuclear Power Reactors[R].BNWL:SA-1529,1968.
[3]S.K.Patil,V.V.Ramakrishna,G.V.N.Avadhnay,M.V.Ramaniah.Neptunium-237 Supply and Demand[J].Proc.Chem.Symp.Bombay,1972,2:275.
[4]D.R.Vondy,J.A.Lane,A.T.Grisky.The Recovery of Neptunium-237 and Plutonium[J].Ind.Eng.Chem.Process Design Develop.1964,3:293.
[5]Ryan J.L.,Wheelwright E.J.Hanford Atomic Products Operation[R].USAEC:HW-55893,Jan.2,1959.
[6]I.L.Jenkins.Separation of Pu-238 from Irradiated Np-237 and Fission Products.I.Preliminary Work[J].Nuclear Science Abstracts,1968,6364:637.
[7]I.L.Jenkins.Separation of Pu-238 from Irradiated Np-237 and Fission Products.II?Processing Runs[J].Nuclear Science Abstracts,1968,6364:637.
[8]Burney,G.A.Recovery of Pu and Np from Irradiated Np-237 Targets[R].USAEC:HW-61145,1959:214-220.
[9]J.Champion.,A.Chesne.L'extraction du neptunium 237 par la trilaurylamineau traitement des Combustibles irradies[R].CEA:R-2607,1971:148-151 USAEC:DP-1023,1965.
[10]李洲,等.液-液萃取过程和设备[M].北京:原子能出版社,1993:1 71-176.
[11]张希祥.萃取法回收提取镎钚的研究[D].北京:中国原子能科学研究院,2006.
[12]吴华武,等.核燃料化学工艺学[M].北京:原子能出版社,1989:225-236.
[13]姜圣阶,任凤仪等.核燃料后处理工学[M].北京:原子能出版社,1995:142-145.
[14]З.N.尼科洛托娃H.A.卡尔塔绍娃,萃取手册第一卷用中性有机化合物的萃取[M].北京:原子能出版社,1981:396-423.
[15]A.A.柴霍尔斯基,邱孝熹译,林漳基校,镎化学[M].北京:原子能出版社,1986.
[16]李小该.APOR流程1B槽中镎的走向行为研究[D].北京:中国原子能科学研究院,2009.