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, 2015, 31(9): 1774-1784. doi: 10.11862/CJIC.2015.245 shu

Citation: 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. Effect of Low-Enriched Uranium Targets Irradiation on Major Fission Elements and Uranium Speciation[J]. Chinese Journal of Inorganic Chemistry, 2015, 31(9): 1774-1784. doi: 10.11862/CJIC.2015.245 shu

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

兰图 ^1,2, ,
刘展翔 ^1, ,
李兴亮 ^1,3, ,
廖家莉 ^{1,
,} ,
罗顺忠 ^3, ,
杨远友 ^1, ,
柴之芳 ^2,4, ,
刘宁 ^1, ,
王东琪 ^{2,
,}

1.
1. 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;
2.
2. 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;
3.
3. 中国工程物理研究院核物理与化学研究所, 绵阳 621900;
4.
4. 苏州大学放射医学及交叉学科研究院(RAD-X), 苏州 215123

通讯作者: 廖家莉,E-mail:liaojiali@scu.edu.cn,Tel:+86-28-85412613;王东琪,E-mail:dwang@ihep.ac.cn,Tel:+86-10-88236606; 廖家莉,E-mail:liaojiali@scu.edu.cn,Tel:+86-28-85412613;王东琪,E-mail:dwang@ihep.ac.cn,Tel:+86-10-88236606

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) (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) (No.J1210004)

国家自然科学基金委员会(No.91026000) (No.91026000)

中国科学院百人计划(No.Y2291810S3)资助项目。 (No.Y2291810S3)

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0.01 mol·L^-1并分别以TcO₄^-、I^-、MoO₄^2-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;铀;裂变元素;辐照

English

Effect of Low-Enriched Uranium Targets Irradiation on Major Fission Elements and Uranium Speciation

1.
1. Key Laboratory of Radiation Physics and Technology(Sichuan University), Ministry of Education;Institute of Nuclear Science and Technology, Sichuan University, Chengdu 610064, China;
2.
2. CAS Key Laboratory of Nuclear Radiation and Nuclear Techniques, Multidisciplinary Initiative Center, Institute of High Energy Physics, Chinese Academy of Sciences, Beijing 100049, China;
3.
3. Institute of Nuclear Physics and Chemistry, China Academy of Engineering Physics, Mianyang, Sichuan 621900, China;
4.
4. School of Radiation Medicine and Interdisciplinary Sciences(RAD-X), Soochow University, Suzhou, Jiangsu 215123, China

Corresponding author: 廖家莉,E-mail:liaojiali@scu.edu.cn,Tel:+86-28-85412613;王东琪,E-mail:dwang@ihep.ac.cn,Tel:+86-10-88236606; 廖家莉,E-mail:liaojiali@scu.edu.cn,Tel:+86-28-85412613;王东琪,E-mail:dwang@ihep.ac.cn,Tel:+86-10-88236606

Received Date: 10 April 2015
Fund Project:
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。

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 pH value 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^-, MoO₄^2-.

Key words:

speciation;CHEMSPEC;uranium;fission element;irradiation

1. [1] Travelli A. Proceeding of the 19th International Meeting on Reduced Enrichment for Research and Test Reactors. Seoul, Korea, 1996:4-8[1] Travelli A. Proceeding of the 19th International Meeting on Reduced Enrichment for Research and Test Reactors. Seoul, Korea, 1996:4-8
2. [2] Matos J E. Proceeding of the 25th International Meeting on Reduced Enrichment for Research and Test Reactors, RERTR-2003. Chicago, Illinois, 2003:1-8[2] Matos J E. Proceeding of the 25th International Meeting on Reduced Enrichment for Research and Test Reactors, RERTR-2003. Chicago, Illinois, 2003:1-8
3. [3] Yanagisawa K, Fujishiro T. J. Nucl. Sci. Technol., 1995,32(10):981-988[3] Yanagisawa K, Fujishiro T. J. Nucl. Sci. Technol., 1995,32(10):981-988
4. [4] Keilser D, Robinson A, Jue J. F, et al. J. Nucl. Mater., 2009, 393(2):311-320[4] Keilser D, Robinson A, Jue J. F, et al. J. Nucl. Mater., 2009, 393(2):311-320
5. [5] Izhutov A L, Alexandrov V V, Novosyolov A Y, et al. Proceedings of International Meeting on RERTR-2010. Lisbon, Portugal, 2010:10-15[5] Izhutov A L, Alexandrov V V, Novosyolov A Y, et al. Proceedings of International Meeting on RERTR-2010. Lisbon, Portugal, 2010:10-15
6. [6] Moore G A, Rabin B H, Jue J F, et al. Proceedings of International Meeting on RERTR-2010. Lisbon, Portugal, 2010:1-5[6] Moore G A, Rabin B H, Jue J F, et al. Proceedings of International Meeting on RERTR-2010. Lisbon, Portugal, 2010:1-5
7. [7] SUN Rong-Xian(孙荣先), XIE Huai-Ying(解怀英). At. Energ. Sci. Technol.(原子能科学技术), 2011,45(7):847-851[7] SUN Rong-Xian(孙荣先), XIE Huai-Ying(解怀英). At. Energ. Sci. Technol.(原子能科学技术), 2011,45(7):847-851
8. [8] KANG Ya-Lun(唐亚伦). At. Energ. Sci. Technol.(原子能科学技术), 2003,37(Suppl.):21-23[8] KANG Ya-Lun(唐亚伦). At. Energ. Sci. Technol.(原子能科学技术), 2003,37(Suppl.):21-23
9. [9] Omar H, Ghazi N, Hainoun A. Prog. Nucl. Energy, 2012,60:140-145[9] Omar H, Ghazi N, Hainoun A. Prog. Nucl. Energy, 2012,60:140-145
10. [10] Bokhari I, Pervez S. Nucl. Eng. Des., 2010,240:123-128[10] Bokhari I, Pervez S. Nucl. Eng. Des., 2010,240:123-128
11. [11] Albarhoum M. Prog. Nucl. Energy, 2010,52:809-812[11] Albarhoum M. Prog. Nucl. Energy, 2010,52:809-812
12. [12] Albarhoum M. Ann. Nucl. Energ., 2010,37:1351-1355[12] Albarhoum M. Ann. Nucl. Energ., 2010,37:1351-1355
13. [13] Albarhoum M. Prog. Nucl. Energy, 2010,52:536-540[13] Albarhoum M. Prog. Nucl. Energy, 2010,52:536-540
14. [14] Mahmaood T, Pervez S, Iqbal M. Ann. Nucl. Energ., 2008, 35:1440-1446[14] Mahmaood T, Pervez S, Iqbal M. Ann. Nucl. Energ., 2008, 35:1440-1446
15. [15] Bokhari I. Ann. Nucl. Energ., 2004,31:1265-1273[15] Bokhari I. Ann. Nucl. Energ., 2004,31:1265-1273
16. [16] KANG Ya-Lun(唐亚伦), ZHANG Ai-Min(张爱民), ZHANG Ying-Chao(张应超). At. Energ. Sci. Technol.(原子能科学技术), 2005,39(Suppl.):99-103[16] KANG Ya-Lun(唐亚伦), ZHANG Ai-Min(张爱民), ZHANG Ying-Chao(张应超). At. Energ. Sci. Technol.(原子能科学技术), 2005,39(Suppl.):99-103
17. [17] Omar H, Ghazi N, Hainoun A. Prog. Nucl. Energy, 2012,60:140-145[17] Omar H, Ghazi N, Hainoun A. Prog. Nucl. Energy, 2012,60:140-145
18. [18] Youker A J, Chung P L, Tkac P, et al. Proceedings of the 1st Annual Mo-99 Topical Meeting. Santa Fe, New Mexico, 2011:1-12[18] Youker A J, Chung P L, Tkac P, et al. Proceedings of the 1st Annual Mo-99 Topical Meeting. Santa Fe, New Mexico, 2011:1-12
19. [19] Leonard R A, Chen L, Mertz C J, et al. Proceeding of the 19th International Enrichment for Research and Testing Reactors Meeting. Seoul, Korea, 1996:6-10[19] Leonard R A, Chen L, Mertz C J, et al. Proceeding of the 19th International Enrichment for Research and Testing Reactors Meeting. Seoul, Korea, 1996:6-10
20. [20] Mahmood T, Iqbal M. Ann. Nucl. Energ., 2012,42:175-178[20] Mahmood T, Iqbal M. Ann. Nucl. Energ., 2012,42:175-178
21. [21] Vandegrift G F, Conner C, Aase S, et al. Proceedings of the 6th International Topical Meeting, Research Reactor Fuel Management (RRFM). Ghent, Belgium, 2002:11-17[21] Vandegrift G F, Conner C, Aase S, et al. Proceedings of the 6th International Topical Meeting, Research Reactor Fuel Management (RRFM). Ghent, Belgium, 2002:11-17
22. [22] Steven C, Arjan J, Kevin E. Eur. J. Nucl. Med. Mol., 2010, 37:1817-1820[22] Steven C, Arjan J, Kevin E. Eur. J. Nucl. Med. Mol., 2010, 37:1817-1820
23. [23] Vandegrift G, Conner C, Hofman G. et al. Ind. Eng. Chem. Res., 2000,39:3140-3145[23] Vandegrift G, Conner C, Hofman G. et al. Ind. Eng. Chem. Res., 2000,39:3140-3145
24. [24] Matthews K, Bowyer T, Saey P, et al. J. Environ. Radioact., 2012,110:1-6[24] Matthews K, Bowyer T, Saey P, et al. J. Environ. Radioact., 2012,110:1-6
25. [25] WANG Xiang-Yun(王祥云), CHEN Tao(陈涛), LIU Chun-Li (刘春立). Sci. China:Ser. B.(中国科学B辑:化学), 2009, 39(11):1551-1562[25] WANG Xiang-Yun(王祥云), CHEN Tao(陈涛), LIU Chun-Li (刘春立). Sci. China:Ser. B.(中国科学B辑:化学), 2009, 39(11):1551-1562
26. [26] ZHU Jian-Bo(朱建波), WANG Xiang-Yun(王祥云), CHEN Tao(陈涛), et al. Sci. China:Chem.(中国科学:化学), 2012, 42(6):856-864[26] ZHU Jian-Bo(朱建波), WANG Xiang-Yun(王祥云), CHEN Tao(陈涛), et al. Sci. China:Chem.(中国科学:化学), 2012, 42(6):856-864
27. [27] CHEN Tao(陈涛), WANG Xiang-Yun(王祥云), TIAN Wen-Yu(田文宇), et al. Acta Phys.-Chim. Sin.(物理化学学报), 2010,26(4):811-816[27] CHEN Tao(陈涛), WANG Xiang-Yun(王祥云), TIAN Wen-Yu(田文宇), et al. Acta Phys.-Chim. Sin.(物理化学学报), 2010,26(4):811-816
28. [28] Korichi S, Bensmaili A. J. Hazard. Mater., 2009,169(1):780-793[28] Korichi S, Bensmaili A. J. Hazard. Mater., 2009,169(1):780-793
29. [29] Markich S. Sci. World J., 2002,2:707-729[29] Markich S. Sci. World J., 2002,2:707-729
30. [30] Clark D, Conradson S, Donohoe R, et al. Inorg. Chem., 1999, 38(7):1456-1466[30] Clark D, Conradson S, Donohoe R, et al. Inorg. Chem., 1999, 38(7):1456-1466
31. [31] Priyadarshini N, Sampath M, Kumar S, et al. J. Radioanal. Nucl. Chem., 2013,298(3):1923-1931[31] Priyadarshini N, Sampath M, Kumar S, et al. J. Radioanal. Nucl. Chem., 2013,298(3):1923-1931
32. [32] Zanonato P, Di Bernardo, Grenthe I. Dalton Trans., 2014,43(6):2378-2383[32] Zanonato P, Di Bernardo, Grenthe I. Dalton Trans., 2014,43(6):2378-2383
33. [33] Li B, Matveev A, Krüger S, et al. Comput. Theo. Chem., 2015, 1051:151-160[33] Li B, Matveev A, Krüger S, et al. Comput. Theo. Chem., 2015, 1051:151-160
34. [34] Vallet V, Wahlgren U, Grenthe I. J. Phys. Chem. A, 2012, 116(50):12373-12380[34] Vallet V, Wahlgren U, Grenthe I. J. Phys. Chem. A, 2012, 116(50):12373-12380
35. [35] Chien W, Anbalagan V, Zandler M, et al. J. Am. Soc. Mass Spectr., 2004,15(6):777-783[35] Chien W, Anbalagan V, Zandler M, et al. J. Am. Soc. Mass Spectr., 2004,15(6):777-783
36. [36] Rios D, Michelini M, Lucena A, et al. Inorg. Chem., 2012, 51(12):6603-6614[36] Rios D, Michelini M, Lucena A, et al. Inorg. Chem., 2012, 51(12):6603-6614
37. [37] Tsushima S, Reich T. Chem. Phys. Lett., 2001,347(1):127-132[37] Tsushima S, Reich T. Chem. Phys. Lett., 2001,347(1):127-132
38. [38] McGrail B, Pianowski L, Burns P. J. Am. Chem. Soc., 2014, 136(13):4797-4800[38] McGrail B, Pianowski L, Burns P. J. Am. Chem. Soc., 2014, 136(13):4797-4800
39. [39] Suleimenov O, Seward T, Hovey J. J. Solution Chem., 2007, 36(9):1093-1102[39] Suleimenov O, Seward T, Hovey J. J. Solution Chem., 2007, 36(9):1093-1102
40. [40] Sieffert N, Wipff G. Dalton Trans., 2015,44:2623-2638[40] Sieffert N, Wipff G. Dalton Trans., 2015,44:2623-2638
41. [41] Kumar N, Seminario J. J. Phys. Chem. A, 2015,119(4):689-703[41] Kumar N, Seminario J. J. Phys. Chem. A, 2015,119(4):689-703
42. [42] KANG Ming-Liang(康明亮), JIANG Mei-Ling(蒋美玲), YANG Zhuan-Wei(杨颛维), et al. J. Nucl. Radiochem.(核化学与放射化学), 2013,35(3):160-166[42] KANG Ming-Liang(康明亮), JIANG Mei-Ling(蒋美玲), YANG Zhuan-Wei(杨颛维), et al. J. Nucl. Radiochem.(核化学与放射化学), 2013,35(3):160-166
43. [43] Balboni E, Morrison J, Wang Z, et al. Geochim. Cosmochim. Acta, 2015,151:133-149[43] Balboni E, Morrison J, Wang Z, et al. Geochim. Cosmochim. Acta, 2015,151:133-149
44. [44] Pan H, Liao W, Wai C, et al. Dalton Trans., 2014,43(28):10713-10718[44] Pan H, Liao W, Wai C, et al. Dalton Trans., 2014,43(28):10713-10718

扫一扫看文章

计量

PDF下载量: 0
文章访问数: 527
HTML全文浏览量: 87

通讯作者: 陈斌, bchen63@163.com

1.
沈阳化工大学材料科学与工程学院沈阳 110142

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

通讯作者: 廖家莉,E-mail:liaojiali@scu.edu.cn,Tel:+86-28-85412613;王东琪,E-mail:dwang@ihep.ac.cn,Tel:+86-10-88236606; 廖家莉,E-mail:liaojiali@scu.edu.cn,Tel:+86-28-85412613;王东琪,E-mail:dwang@ihep.ac.cn,Tel:+86-10-88236606

English

Effect of Low-Enriched Uranium Targets Irradiation on Major Fission Elements and Uranium Speciation

Corresponding author: 廖家莉,E-mail:liaojiali@scu.edu.cn,Tel:+86-28-85412613;王东琪,E-mail:dwang@ihep.ac.cn,Tel:+86-10-88236606; 廖家莉,E-mail:liaojiali@scu.edu.cn,Tel:+86-28-85412613;王东琪,E-mail:dwang@ihep.ac.cn,Tel:+86-10-88236606

CCS Chemistry：嵌段共聚物自组装成 “三明治”二维有机材料，实现纳米级压力传感功能

CCS Chemistry：颜徐州、鲍哲南：你的皮肤可能是一片SPMs

CCS Chemistry：工作高效不疲劳，只须让催化剂动起来

CCS Chemistry：静电组装导向聚合- 聚电解质纳米凝胶量化制备新策略

CCS Chemistry：金黄色葡萄球菌醛基脱氢酶是如何识别特异性底物的？

计量

通讯作者: 陈斌, bchen63@163.com

中国化学会秘书处

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

通讯作者: 廖家莉,E-mail:liaojiali@scu.edu.cn,Tel:+86-28-85412613;王东琪,E-mail:dwang@ihep.ac.cn,Tel:+86-10-88236606; 廖家莉,E-mail:liaojiali@scu.edu.cn,Tel:+86-28-85412613;王东琪,E-mail:dwang@ihep.ac.cn,Tel:+86-10-88236606

English

Effect of Low-Enriched Uranium Targets Irradiation on Major Fission Elements and Uranium Speciation

Corresponding author: 廖家莉,E-mail:liaojiali@scu.edu.cn,Tel:+86-28-85412613;王东琪,E-mail:dwang@ihep.ac.cn,Tel:+86-10-88236606; 廖家莉,E-mail:liaojiali@scu.edu.cn,Tel:+86-28-85412613;王东琪,E-mail:dwang@ihep.ac.cn,Tel:+86-10-88236606

CCS Chemistry：嵌段共聚物自组装成 “三明治”二维有机材料，实现纳米级压力传感功能

CCS Chemistry：颜徐州、鲍哲南： 你的皮肤可能是一片SPMs

CCS Chemistry：工作高效不疲劳，只须让催化剂动起来

CCS Chemistry：静电组装导向聚合- 聚电解质纳米凝胶量化制备新策略

CCS Chemistry：金黄色葡萄球菌醛基脱氢酶是如何识别特异性底物的？

计量

文章相关

通讯作者: 陈斌, bchen63@163.com

中国化学会秘书处

CCS Chemistry：颜徐州、鲍哲南：你的皮肤可能是一片SPMs