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2021 , Vol. 79 >Issue 12: 1425 - 1437

DOI: https://doi.org/10.6023/A21070341

综述

氯化物熔盐体系中铀的化学种态研究进展

  • 刘毅川 ,
  • 刘雅兰 ,
  • 姜仕林 ,
  • 李梅 ,
  • 石伟群
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  • a 哈尔滨工程大学 材料科学与化学工程学院 哈尔滨 150001
    b 中国科学院高能物理研究所 北京 100049

刘毅川,哈尔滨工程大学博士研究生,主要从事熔盐中锕系镧系化学研究.

刘雅兰, 中国科学院高能物理研究所副研究员, 研究方向为锕系镧系熔盐化学, 多年来致力于氧化物乏燃料干法后处理领域, 聚焦于锕-镧分离研究. 首先开展了锕、镧系氧化物在熔盐中的溶解及其电化学行为研究, 随后在固态活性铝阴极上进行了锕-镧的电化学分离, 并采用原位光谱技术监测了分离过程中锕、镧元素的化学种态变化, 发现了铀的循环电解并将其消除, 提高了电流效率. 最终成功实现了锕-镧元素的有效分离, 与传统的液态Cd阴极相比将分离因子提高了两个数量级. 在此基础上, 进一步总结了锕、镧氧化物在氯化物熔盐中的溶解规律, 提出了利用其溶解性差异实现一步分离的新方法. 基于相关工作,在电化学领域与核能领域著名期刊Electrochim. Acta, J. Electrochem. Soc., Electrochem. Commun.和J. Nucl. Mater.等上共发表论文40余篇, 其中第一作者及通讯作者论文20篇.

姜仕林, 中国科学院高能物理研究所博士研究生, 主要从事锕系镧系熔盐电化学研究.

李梅, 哈尔滨工程大学教授, 国家自然科学基金通讯评审专家, 教育部学位与研究生教育评估专家. Electrochimica Acta, Journal of The Electrochemical Society, Journal of Alloys and Compounds, Journal of Nuclear Materials, ACS inoganic Chemistry, ACS Sustainable Chemistry & Engineering等国际期刊审稿人. 近来年发表SCI检索论文60余篇, 其中以第一/通讯作者在Electrochimica Acta, Journal of The Electrochemical Society, Journal of Nuclear Materials, Journal of Alloys and Compounds, RSC Advances等期刊上发表SCI收录论文40余篇. 申请专利12项, 获授权发明专利6项, 获省部级二等奖1项.

石伟群, 中国科学院高能物理研究所研究员, 国家杰出青年科学基金获得者, 长期致力于核燃料循环化学与锕系元素化学相关基础研究, 在JACS, Angew. Chem., Chem, CCS Chem., Nat. Commun, Adv. Mater., Environ. Sci. Technol.等国际知名期刊发表SCI论文200余篇, 成果被国内外同行广泛关注和引用, 文章总引8000余次, H因子46 (Google Scholar). 分别担任英文期刊Journal of Nuclear Fuel Cycle and Waste Technology和Journal of Nuclear Science and Technology的编委与国际顾问编委, 中文期刊《核化学与放射化学》编委. 现为中国化学会核化学与放射化学专业委员会委员、中国核学会锕系物理与化学分会副理事长、中国有色金属学会熔盐化学与技术专业委员会副主任委员、中国核学会核化工分会理事兼副秘书长.

收稿日期: 2021-07-23

  网络出版日期: 2021-09-14

基金资助

国家杰出青年科学基金(21925603); 国家自然科学基金重大项目(21790373); 国家自然科学基金(U20B2020)

收起

Recent Progress on Chemical Species of Uranium in Molten Chlorides

  • Yichuan Liu ,
  • Yalan Liu ,
  • Shilin Jiang ,
  • Mei Li ,
  • Weiqun Shi
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  • a College of Material Science and Chemical Engineering, Harbin Engineering University, Harbin 150001, China
    b Institute of High Energy Physics, Chinese Academy of Sciences, Beijing 100049, China
* E-mail: ;
; Tel.: 010-88233989; Fax: 010-88235294

Received date: 2021-07-23

  Online published: 2021-09-14

Supported by

National Science Fund for Distinguished Young Scholars(21925603); Major Program of the National Natural Science Foundation of China(21790373); National Natural Science Foundation of China(U20B2020)

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摘要

乏燃料后处理是未来先进核燃料循环体系的中心环节, 基于高温熔盐电解的干法后处理技术具有一定优势. 该技术通常在高温氯化物熔盐体系中进行, 采用电化学技术回收锕系元素, 并实现其与镧系元素的电解分离. 其中铀的分离回收是研究的重点之一. 为更好实现铀在熔盐中的分离与回收, 需要深入理解铀的电化学性质与其在熔盐中的配位化学性质的联系. 因此, 开展铀在氯盐体系中的化学种态研究至关重要. 本Review对国际上氯化物熔盐体系中针对铀化学种态的研究进展进行了总结归纳和提炼, 并对未来锕系元素在高温熔盐介质中的化学种态研究进行了展望.

关键词： 干法后处理; 熔盐; 化学种态; 铀

本文引用格式

刘毅川 , 刘雅兰 , 姜仕林 , 李梅 , 石伟群 . 氯化物熔盐体系中铀的化学种态研究进展[J]. 化学学报, 2021 , 79(12) : 1425 -1437 . DOI: 10.6023/A21070341

Abstract

High-temperature molten salt electrolysis based pyrochemical reprocessing of spent nuclear fuel has certain advantages for advanced nuclear fuel cycle, which is usually carried out in a high-temperature chloride molten salt system, and actinides (Ans) are recovered and separated over lanthanides (Lns) via electrolysis in molten salt. Among them, the separation and recovery of uranium from fission products (FPs) is one of the key tasks. To optimize the separation process, it is necessary to deeply understand the relationship between electrochemical properties and chemical species of uranium in molten salt. Hence, it is very important to carry out the study of the chemical species of uranium in molten chlorides. In this review, the research progresses on chemical species of uranium in molten chlorides have been summarized and sorted. In addition, future perspectives upon actinide chemical species in molten salt have been given.

Key words： pyrochemical reprocessing; molten salt; chemical species; uranium

参考文献

[1]
Glatz, J. P.; Malmbeck, R.; Souček, P.; Claux, B.; Meier, R.; Ougier, M.; Murakami, T. Molten Salts Chemistry, Elsevier, Amsterdam, 2013, pp. 541-560.
[2]
Inoue, T.; Koch, L. Nucl. Eng. Technol. 2008, 40, 183.
[3]
Hoover, R. O.; Shaltry, M. R.; Martin, S.; Sridharan, K.; Phongikaroon, S. J. Nucl. Mater. 2014, 452, 389.
[4]
Salanne, M.; Simon, C.; Turq, P.; Madden, P. A. J. Phys. Chem. B 2008, 112, 1177.
[5]
Masset, P.; Bottomley, D.; Konings, R.; Malmbeck, R.; Rodrigues, A.; Serp, J.; Glatz, J.-P. J. Electrochem. Soc. 2005, 152, A1109.
[6]
Shirai, O.; Iwai, T.; Suzuki, Y.; Sakamura, Y.; Tanaka, H. J. Alloys Compd. 1998, 271, 685.
[7]
Yin, T.; Liu, K.; Liu, Y.; Yan, Y.; Wang, G.; Chai, Z.; Shi, W. J. Electrochem. Soc. 2018, 165, D722.
[8]
Yang, D. W.; Liu, Y. L.; Yin, T. Q.; Jiang, S. L.; Zhong, Y. K.; Wang, L.; Li, M.; Chai, Z. F.; Shi, W. Q. Electrochim. Acta 2020, 353, 136449.
[9]
Salanne, M.; Simon, C.; Turq, P.; Ohtori, N.; Madden, P. A. Molten Salts Chemistry, Elsevier, Amsterdam, 2013, pp. 1-16.
[10]
Li, X.; Song, J.; Shi, S.; Yan, L.; Zhang, Z.; Jiang, T.; Peng, S. J. Phys. Chem. A 2017, 121, 571.
[11]
Kwon, C.; Kang, J.; Han, B. Int. J. Energ. Res. 2016, 40, 1381.
[12]
Dai, S.; Toth, L. M.; Del Cul, G. D.; Metcalf, D. H. J. Phys. Chem. 1996, 100, 220.
[13]
Polovov, I. B.; Volkovich, V. A.; Charnock, J. M.; Kralj, B.; Lewin, R. G.; Kinoshita, H.; May, I.; Sharrad, C. A. Inorg. Chem. 2008, 47, 7474.
[14]
Volkovich, V. A.; Bhatt, A. I.; May, I.; Griffiths, T. R.; Thied, R. C. J. Nucl. Sci. Technol. 2014, 39, 595.
[15]
Nagai, T.; Uehara, A.; Fujii, T.; Shirai, O.; Sato, N.; Yamana, H. J. Nucl. Sci. Technol. 2005, 42, 1025.
[16]
May, I. ECS Proceedings Volumes, 2004, 2004-24, 814.
[17]
Volkovich, V. A.; May, I.; Griffiths, T. R.; Charnock, J. M.; Bhatt, A. I.; Lewin, B. J. Nucl. Mater. 2005, 344, 100.
[18]
Volkovich, V. A.; Aleksandrov, D. E.; Vasin, B. D.; Khabibullin, T. K.; Polovov, I. B.; Griffiths, T. R. ECS Trans. 2009, 16, 325.
[19]
Nagai, T.; Fujii, T.; Shirai, O.; Yamana, H. J. Nucl. Sci. Technol. 2004, 41, 690.
[20]
Fujii, T.; Moriyama, H.; Yamana, H. J. Alloys Compd. 2003, 351, L6.
[21]
Fujii, T.; Nagai, T.; Sato, N.; Shirai, O.; Yamana, H. J. Alloys Compd. 2005, 393, L1.
[22]
Fujii, T.; Nagai, T.; Uehara, A.; Yamana, H. J. Alloys Compd. 2007, 441, L10.
[23]
Kim, T. J.; Jeong, Y. K.; Kang, J. G.; Jung, Y.; Ahn, D. H.; Lee, H. S. J. Radioanal. Nucl. Chem. 2010, 286, 283.
[24]
Volkovich, V. A.; Polovov, I. B.; Vasin, B. D.; Griffiths, T. R.; Sharrad, C. A.; May, I.; Charnock, J. M. Zeitschrift für Naturforschung A 2007, 62, 671.
[25]
Fujii, T.; Uda, T.; Iwadate, Y.; Nagai, T.; Uehara, A.; Yamana, H. J. Nucl. Mater. 2013, 440, 575.
[26]
Preetz, W.; Ruf, D.; Tensfeldt, D. Zeitschrift für Naturforschung B 1984, 39, 1100.
[27]
Kwon, C.; Kang, J.; Kang, W.; Kwak, D.; Han, B. Electrochim. Acta 2016, 195, 216.
[28]
Till, C.; Chang, Y.; Hannum, W. Prog. Nucl. Energ. 1997, 31, 3.
[29]
Karell, E. J.; Gourishankar, K. V.; Smith, J. L.; Chow, L. S.; Redey, L. Nucl. Technol. 2001, 136, 342.
[30]
Simpson, M. F. Developments of spent nuclear fuel pyroprocessing technology at Idaho National Laboratory, Idaho National Laboratory (INL), 2012.
[31]
Gruen, D.; McBeth, R. J. Inorg. Nucl. Chem. 1959, 9, 290.
[32]
Wenz, D. A.; Adams, M. D.; Steunenberg, R. K. Inorg. Chem. 1964, 3, 989.
[33]
Adams, M.; Wenz, D.; Steunenberg, R. J. Phys. Chem. 1963, 67, 1939.
[34]
Li, B.; Dai, S.; Jiang, D. E. ACS Appl. Energ. Mater. 2019, 2, 2122.
[35]
Li, B.; Dai, S.; Jiang, D. E. J. Mol. Liq. 2020, 299, 112184.
[36]
Wu, F.; Roy, S.; Ivanov, A. S.; Gill, S. K.; Topsakal, M.; Dooryhee, E.; Abeykoon, M.; Kwon, G.; Gallington, L. C.; Halstenberg, P.; Layne, B.; Ishii, Y.; Mahurin, S. M.; Dai, S.; Bryantsev, V. S.; Margulis, C. J. J. Phys. Chem. Lett. 2019, 10, 7603.
[37]
Okamoto, Y.; Kobayashi, F.; Ogawa, T. J. Alloys Compd. 1998, 271, 355.
[38]
Okamoto, Y.; Madden, P. A.; Minato, K. J. Nucl. Mater. 2005, 344, 109.
[39]
Okamoto, Y.; Akabori, M.; Itoh, A.; Ogawa, T. J. Nucl. Sci. Technol. 2014, 39, 638.
[40]
In ACTINIDES 2009, IOP Conference Series: Materials Science and Engineering, Vol. 9, Eds.: Rao, L.; Tobin, J. G.; Shuh, D. K., IOP publishing, Bristol, 2010, p. 012050.
[41]
Fujii, T.; Uehara, A.; Nagai, T.; Kim, T.-J.; Sato, N.; Sakamura, Y.; Yamana, H. Electrochemistry 2009, 77, 667.
[42]
Nagai, T.; Uehara, A.; Fujii, T.; Sato, N.; Yamana, H. J. Nucl. Mater. 2011, 414, 226.
[43]
Nagai, T.; Uehara, A.; Fujii, T.; Yamana, H. J. Nucl. Mater. 2013, 439, 1.
[44]
Fujii, T. KURRI Progress Report 2016, 2015(APRIL 2015-MARCH 2016), 24.
[45]
Choi, E. Y.; Jeon, M. K.; Hur, J.-M. J. Radioanal. Nucl. Chem. 2017, 314, 207.
[46]
Choi, E. Y.; Lee, J. J. Nucl. Mater. 2017, 494, 439.
[47]
Choi, E. Y.; Lee, J.; Heo, D. H.; Lee, S. K.; Jeon, M. K.; Hong, S. S.; Kim, S. W.; Kang, H. W.; Jeon, S. C.; Hur, J. M. J. Nucl. Mater. 2017, 489, 1.
[48]
Cho, Y. H.; Bae, S. E.; Kim, D. H.; Park, T. H.; Kim, J. Y.; Song, K.; Yeon, J. W. Microchem. J. 2015, 122, 33.
[49]
Park, Y. J.; Bae, S. E.; Cho, Y. H.; Kim, J. Y.; Song, K. Microchem. J. 2011, 99, 170.
[50]
Cho, Y. H.; Bae, S. E.; Park, Y. J.; Oh, S. Y.; Kim, J. Y.; Song, K. Microchem. J. 2012, 102, 18.
[51]
Volkovich, V. A.; Griffiths, T. R.; Fray, D. J.; Thied, R. C. Phys. Chem. Chem. Phys. 2000, 2, 3871.
[52]
Bhatt, A. I.; du Fou de Kerdaniel, E.; Kinoshita, H.; Livens, F. R.; May, I.; Polovov, I. B.; Sharrad, C. A.; Volkovich, V. A.; Charnock, J. M.; Lewin, R. G. Inorg. Chem. 2005, 44, 2.
[53]
Volkovich, V.; Aleksandrov, D.; Maltsev, D.; Vasin, B.; Polovov, I.; Griffiths, T. Molten Salts Chemistry and Technology, John Wiley & Sons, New Jersey, 2014, pp. 507-520.
[54]
Volkovich, V. A.; Aleksandrov, D. E.; Griffiths, T. R.; Vasin, B. D.; Khabibullin, T. K.; Maltsev, D. S. Pure Appl. Chem. 2010, 82, 1701.
[55]
Volkovich, V. A.; Aleksandrov, D. E.; Vasin, B. D.; Maltsev, D. S.; Griffiths, T. R. ECS Trans. 2010, 33, 371.
[56]
Polovov, I. B.; Sharrad, C. A.; May, I.; Vasin, B. D.; Volkovich, V. A.; Griffiths, T. R. ECS Trans. 2007, 3, 503.
[57]
Jiang, T.; Wang, N.; Peng, S.; Yan, L. Chem. Res. Chin. Univ. 2015, 31, 281.
[58]
Liu, Y. L.; Yuan, L. Y.; Zheng, L. R.; Wang, L.; Yao, B. L.; Chai, Z. F.; Shi, W. Q. Electrochem. Commun. 2019, 103, 55.
[59]
Song, J.; Shi, S.; Li, X.; Yan, L. J. Mol. Liq. 2017, 234, 279.
[60]
Liu, Y. L.; Luo, L. X.; Liu, N.; Yao, B. L.; Liu, K.; Yuan, L. Y.; Chai, Z. F.; Shi, W. Q. J. Nucl. Mater. 2018, 508, 63.
[61]
Liu, Y. C.; Liu, Y. L.; Wang L.; Zhong Y. K.; Li M.; Han W.; Zhao Y.; Zhou T.; Zou Q.; Zeng X.; Shi W. Q. J. Nucl. Mater. 2020, 542, 152475.
[62]
Liu Y. C.; Liu Y. L.; Zhao Y.; Liu Z.; Zhou T.; Zou Q.; Zeng X.; Zhong Y. K.; Li M.; Sun Z. X.; Shi W. Q. J. Nucl. Mater. 2020, 532, 152049.
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