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低浓缩铀靶辐照后溶液中铀的化学种态及主要裂变元素的影响
引用本文:兰图,刘展翔,李兴亮,廖家莉,罗顺忠,杨远友,柴之芳,刘宁,王东琪. 低浓缩铀靶辐照后溶液中铀的化学种态及主要裂变元素的影响[J]. 无机化学学报, 2013, 29(18)
作者姓名:兰图  刘展翔  李兴亮  廖家莉  罗顺忠  杨远友  柴之芳  刘宁  王东琪
作者单位:四川大学原子核科学技术研究所, 辐射物理及技术教育部重点实验室, 成都 610064;中国科学院核辐射与核技术重点实验室, 中国科学院高能物理研究所多学科中心, 北京 100049,四川大学原子核科学技术研究所, 辐射物理及技术教育部重点实验室, 成都 610064,四川大学原子核科学技术研究所, 辐射物理及技术教育部重点实验室, 成都 610064;中国工程物理研究院核物理与化学研究所, 绵阳 621900,四川大学原子核科学技术研究所, 辐射物理及技术教育部重点实验室, 成都 610064,中国工程物理研究院核物理与化学研究所, 绵阳 621900,四川大学原子核科学技术研究所, 辐射物理及技术教育部重点实验室, 成都 610064,中国科学院核辐射与核技术重点实验室, 中国科学院高能物理研究所多学科中心, 北京 100049;苏州大学放射医学及交叉学科研究院(RAD-X), 苏州 215123,四川大学原子核科学技术研究所, 辐射物理及技术教育部重点实验室, 成都 610064,中国科学院核辐射与核技术重点实验室, 中国科学院高能物理研究所多学科中心, 北京 100049
基金项目:国家自然科学基金委员会和中国工程物理研究院联合基金(NSAF,No.U1330125)、国家基础科学人才培养基金·特殊学科点资助项目(No.J1210004)、国家自然科学基金委员会(No.91026000)、中国科学院百人计划(No.Y2291810S3)资助项目。
摘    要:利用化学种态分析软件CHEMSPEC计算了低浓缩铀靶辐照后溶液中铀(U)的化学种态分布及其主要裂变元素对U化学种态的影响。结果表明,在单组分体系中,pH值和铀酰浓度都会显著影响U的化学种态分布。随着铀酰浓度的增大,溶液中将会生成多核配合物;在较高的NO3-浓度下,U在溶液中主要以UO22+和UO2NO3+的形式存在。CO2对不同浓度铀的种态分布影响结果表明,当铀酰浓度较低时,铀的化学种态多以碳酸铀酰的形式存在;当铀酰浓度较高时,铀的化学种态多以氢氧铀酰或柱铀矿沉淀的形式存在。计算发现,当裂片元素Tc、I、Mo的浓度小于0.01mol·L-1并分别以TcO4-、I-、MoO42-的种态存在时,这些裂片元素不改变铀的各化学种态的分布。

关 键 词:化学种态  CHEMSPEC    裂变元素  辐照

Effect of Low-Enriched Uranium Targets Irradiation on Major Fission Elements and Uranium Speciation
LAN Tu,LIU Zhan-Xiang,LI Xing-Liang,LIAO Jia-Li,LUO Shun-Zhong,YANG Yuan-You,CHAI Zhi-Fang,LIU Ning and WANG Dong-Qi. Effect of Low-Enriched Uranium Targets Irradiation on Major Fission Elements and Uranium Speciation[J]. Chinese Journal of Inorganic Chemistry, 2013, 29(18)
Authors:LAN Tu  LIU Zhan-Xiang  LI Xing-Liang  LIAO Jia-Li  LUO Shun-Zhong  YANG Yuan-You  CHAI Zhi-Fang  LIU Ning  WANG Dong-Qi
Affiliation:Key Laboratory of Radiation Physics and Technology (Sichuan University), Ministry of Education; Institute of Nuclear Science and Technology, Sichuan University, Chengdu 610064, China;CAS Key Laboratory of Nuclear Radiation and Nuclear Techniques, Multidisciplinary Initiative Center, Institute of High Energy Physics, Chinese Academy of Sciences, Beijing 100049, China,Key Laboratory of Radiation Physics and Technology (Sichuan University), Ministry of Education; Institute of Nuclear Science and Technology, Sichuan University, Chengdu 610064, China,Key Laboratory of Radiation Physics and Technology (Sichuan University), Ministry of Education; Institute of Nuclear Science and Technology, Sichuan University, Chengdu 610064, China;Institute of Nuclear Physics and Chemistry, China Academy of Engineering Physics, Mianyang, Sichuan 621900, China,Key Laboratory of Radiation Physics and Technology (Sichuan University), Ministry of Education; Institute of Nuclear Science and Technology, Sichuan University, Chengdu 610064, China,Institute of Nuclear Physics and Chemistry, China Academy of Engineering Physics, Mianyang, Sichuan 621900, China,Key Laboratory of Radiation Physics and Technology (Sichuan University), Ministry of Education; Institute of Nuclear Science and Technology, Sichuan University, Chengdu 610064, China,CAS Key Laboratory of Nuclear Radiation and Nuclear Techniques, Multidisciplinary Initiative Center, Institute of High Energy Physics, Chinese Academy of Sciences, Beijing 100049, China;School of Radiation Medicine and Interdisciplinary Sciences (RAD-X), Soochow University, Suzhou 215123, China,Key Laboratory of Radiation Physics and Technology (Sichuan University), Ministry of Education; Institute of Nuclear Science and Technology, Sichuan University, Chengdu 610064, China and CAS Key Laboratory of Nuclear Radiation and Nuclear Techniques, Multidisciplinary Initiative Center, Institute of High Energy Physics, Chinese Academy of Sciences, Beijing 100049, China
Abstract:The speciation of uranium and effect of major fission products after low-enriched uranium targets being irradiated and solvated were analyzed using the geochemical program CHEMSPEC. The results indicate that the speciation of uranium in water is determined by pHvalue and the concentration of uranyl, and polynuclear complexes may be generated at high concentration of uranyl. Nitrate anion in the solution may interact with uranyl, and at high concentration of nitrate, uranyl exists as UO22+ and UO2NO3+. The presence of CO2 at low concentrations of uranium brings substantial distribution uranyl carbonate, while this is negligible at high concentration of uranyl due to heavy hydrolysis and aggregation of uranyl. The calculations also show that the major fission products, Tc, I, and Mo, do not affect the speciation of uranium when their concentrations are below 0.01 mol·L-1 and when they exist as TcO4-, I-, MoO42-.
Keywords:speciation  CHEMSPEC  uranium  fission element  irradiation
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