中文
Earlier issues
Announcement
More
Progress in Chemistry 2011, Vol. 23 Issue (7): 1272-1288 Previous Articles   Next Articles

• Special issues •

Progress and Discussion on Chemical Separation Technologies for Nuclear Fuel Reprocessing Abroad

Wei Yuezhou   

  1. School of Nuclear Science and Engineering, Shanghai Jiao Tong University, Shanghai 200240, China
  • Received: Revised: Online: Published:
PDF ( 3399 ) Cited
Export

EndNote

Ris

BibTeX

Reprocessing technologies can be divided into wet process using aqueous solution and dry process. The wet process includes solvent extraction (liquid-liquid extraction), ion exchange, precipitation, etc. The PUREX process which uses TBP as extractant and can recover about 99.5% of the U and Pu from spent fuel is the only successfully commercialized reprocessing technology nowadays.However, the PUREX process still has some significant drawbacks such as complicated extraction procedures, generation of a great amount of waste and utilization of large scale equipment. In addition, it can not effectively recover the long-lived nuclides such as minor actinides (Np, Am, Cm) and Tc, which will result in a long term radiological effect on the environment. In recent years, many efforts have been devoted to the improvement of the PUREX process and the study of advanced wet reprocessing technologies. Dry process utilizing electro-refining in molten salt, reductive extraction in liquid metal or volatilization of fluorides is attracting wide attention, because it has the advantages of compact equipment, high radiation resistance and critical safety. But relatively low separation factor and corrosion of materials at high temperature are the main problems of the dry process. This article reviews the progress in the chemical separation technologies for nuclear fuel reprocessing abroad. Furthermore, some chemical problems in separation processes are analyzed and discussed.

Contents
1 Necessity for the development of advanced reprocessing technologies
2 Progress and discussion on advanced wet reprocessing technologies
2.1 Extraction processes based on the improvement of PUREX
2.2 Separation processes using novel extractants
2.3 Other wet separation processes
2.4 Separation processes for MA and FP
2.5 Summary of wet separation processes
3 Progress and discussion on dry reprocessing technologies
3.1 The principle and characteristics of dry separation processes
3.2 Molten salt electro-refining process for metalic nuclear fuel
3.3 Molten salt electro-reduction process for oxide nuclear fuel
3.4 Hybrid process of dry and wet separation technologies
3.5 Summary of dry separation processes
4 Concluding remarks

Key words: spent nuclear fuel, chemical separation, wet reprocessing, dry reprocessing

CLC Number: 


[1] Benedict M, Pigford T H, Levi H W. Nuclear Chemical Engineering(2nd Edition), 1981, McGraw-Hill

[2] Takahashi K. Analysis and Study of Spent Fuel Reprocessing Technology from Birth to Present, Ronbunshi of Atomic Energy Society of Japan, 2006, 5 (2): 152-165 (in Japanese)

[3] Research Organization for Information Science & Technology. Gensiryokuhyakkajiten ATOMICA, http://www.rist.or.jp/atomica/ (in Japanese)

[4] ISIS (Institute for Science and International Security), Status and Stocks of Military Plutonium in the Acknowledged Nuclear Weapon States, (2004), http://www.isis-online.org

[5] Nuclear Weapon Archive, France's Nuclear Weapons: French Nuclear Facilities. Marcoule (2001), http://nuclearweaponarchive.org

[6] Suzuki A. Plutonium, The University of Tokyo Publisher, 1994 (in Japanese)

[7] Yu H, Hu Y. Fuel Cycle inside FBR, Studies on Development Strategy of Nuclear Fuel Cycle in China (Consulting report of the Chinese Academy of Science), 2010 (in Chinese)

[8] Akimoto Y. Subjects in Nuclear Policies Faced by Japan, The Lecture at Kansai Electric Power Company. 6 July, 2005 (in Japanese)

[9] Wei Y Z, Arai T, Kumagai M. A Study on FBR fuel Reprocessing by Ion Exchange Method, JNC TJ9400 2000-002 (in Japanese)

[10] Atomic Energy Society of Japan. Overview of Partitioning and Transmutation Technology Development, Chapter 4, 2004 (in Japanese)

[11] IAEA: Spent Fuel Reprocessing Options, IAEA-TECDOC-1587(2008)

[12] Research Committee on Partitioning and Transmutation Cycle of AESJ. Status and Perspectives of Partitioning and Transmutation Technology. Journal of AESJ, 2008(3) 158-163 (in Japanese)

[13] A Report of Japan Atomic Energy Commission Attached papers: http://www.aec.go.jp/jicst/NC/ senmon/bunri/siryo/bunri03/siryo2-2.pdf (in Japanese)

[14] Uchiyama G, Hotoku S, Fujine S, Maeda M. Nucl.Technol.,1998,122(2): 222-227

[15] Todd T A, Felker L K, Vienna J D, Bresee J, Lesica S. The Advanced Fuel Cycle Initiative Separations and Waste Campaign: Accomplishments and Strategy, Proceedings of GLOBAL 2009. Paris, Sep. 8-11, 2009, 9111

[16] Phillips C, Arm S, Banfield Z, Taylor R. Use of Pilot Plants for Developing used Nuclear Fuel Recycling Facilkities. Proceedings of GLOBAL 2009. Paris, Sep. 8- NFDB3 11 2009, 9509

[17] Nash K L, Grimes T S, Nilsson M. Fundamental Studies of TALSPEAK Chemistry for Trivalent Actinide- NFDB3 Lanthanide Separations in Advanced Nuclear Fuel Cycles. Proceedings of GLOBAL 2009. Paris, Sep. 8-11, 2009, 9457

[18] Board of Inquiry Report:Fractured Pipe with Loss of Primary Containment in the THORP Feed Clarication Cell, BNFL,May 2005, http://www.britishnucleargroup.com/

[19] Nakahara M, Sano Y, Koizumi T. U, Pu and Np Co-recovery in Simplified Solvent Extraction Process, JAEA-Research 2008-078 (in Japanese)

[20] Tachimori S. ARTIST Process: A Novel Chemical Process for Treatment of Spent Nuclear Fuel, JAEA-Research 2001-048 (in Japanese)

[21] Tachimori S, Suzuki S, Sasaki Y. Journal of AESJ, 2001, 43(12): 1235 (in Japanese)

[22] Tachimori S, Sasaki Y, Suzuki S. Solvent Extr. Ion Exch.,2002,20(6):687-699

[23] CEA Textbook: Le Traitement-Recyclage du Combustible Nucleaire Use. 2008

[24] Warin D, Poinssot C, Baron P, Lorrain B. Advanced processes for Actinide Partitioning: Recent Experiments and Results, Proceedings of GLOBAL 2009. Paris, Sep. 8-11 2009, Paper 9531

[25] Miguirditchian M, Sorel C, Camès B, Bisel I, Baron P, Espinoux D, Calor J N, Viallesoubranne C, Lorrain B, Masson M. HA Demonstration in the Atalante Facility of the Ganex 1st Cycle for the Selective Extraction of Uranium from HLW, Proceedings of GLOBAL 2009. Paris, Sep. 8-11 2009, 9377

[26] Wei Y Z, Kumagai M, Takashima Y, Bruggeman A, Gyseman M. J. Nucl. Sci. Technol., 1999,36 :304-306

[27] Wei Y Z, Kumagai M, Takashima Y, Sawa T, Bruggeman A, Gyseman M. An Advanced Ion Exchange Process for Reprocessing Spent Nuclear Fuels-Separation of Real Spent Fuel Solutions and Conceptual Design of the Process, Proc. Global 2001, Paris, Sep. 8-11, 2001,003

[28] Wei Y Z. J. Ion Exchange, 2005,16(2) :102-114

[29] Ikeda Y, Wada E, Harada M, Chikazawa T, Kikuchi T, Mineo H, Morita Y, Nogami M, Suzuki K. J. Alloys Comp., 2004,374 :420-425

[30] Y. Morita, Morita Y, Kawata Y, Mineo H, Koshino N,Asanuma N, Ikeda Y,Yamasaki K, Chikazawa T, Tamaki Y, Kikuchi T. J. Nucl. Sci. Technol., 2007,44:354-360

[31] Takaki N, Shinoda Y, Watanabe M, Yoshida K. ORIENT-CYCLE-Evolutional Recycle Concept with Fast Reactor for Minimizing High-Level Waste, Proc. of The Seventh Information Exchange Meeting on Actinide and Fission Product Partitioning &Transmutation,Oct.14-16,2002, Korea,2003

[32] Koyama S, Ozawa M. Advanced ORIENT Cycle Study (Phase I) (8) Summary and prospect, Proceedings of 2010 Fall Meeting of Atomic Energy Society of Japan (in Japanese)

[33] Shimada T, et al. Development on Direct Extraction of Uranium and Plutonium from Spent Fuel by Super-DIREX Reprocessing Method (19), Proceedings of 2005 Spring Meeting of Atomic Energy Society of Japan (in Japanese)

[34] Suyama K, Shimada T, Ishihara N, Kuroda K, Mori Y, Ishida Y. Development of Nuclear Fuel Recycle System by using Supercritical Fluid Carbon Dioxide for the Transition Period from LWR to FBR, Global 2009, Paris, 2009. 9385

[35] Horwitza E P, Kalinaa D C, Diamonda H, Vandegrifta G F, Schulzb W W.Solvent Extr. Ion Exch., 1985,3(1/2):75-109

[36] Weaver B, Kappelmann F A. TALSPEAK: A New Method of Separating Americium and Curium from the Lanthanides by Extraction from an Aqueous Solution of an Aminopolyacetic Acid with a Monoacidic Organophosphate or Phosphonate,ORNL-3559,1964

[37] Madic C, Blanc P, et al. Actinide Partitioning from High Level Liquid Waste Using the Diamex Process”,Proc.of Record ’94, 1994, vol.3 (poster session:actinide separation)

[38] Baron P, Heres X, Lecomte M, Masson M.Separation of the Actinides: the DIAMEX-SANEX Concept,Proc. of Global 2001,2001

[39] Rostaing C, Baron P, Warin D, Duhamet J, Ochem D.Advanced processes for minor actinides recycling: studies towards potential industrialization, Proceedings of GLOBAL 2009,Paris,2009. 9380

[40] Pochon P, Sans D, Lartigaud C, Bisel I.Management of high level radioactive aqueous effluents in advanced partitioning process, Proceedings of GLOBAL 2009,Paris, 2009. 9114

[41] Morita Y, Yamaguchi I, Fujiwara T, Mizoguchi K, Kubota M. Cold and Semi-Hot Tests of 4-Group Partitioning Process at NUCE F, JAERI-Research, 2000, 2000-24 (in Japanese)

[42] Kubota M, Morita Y. Preliminary Assessment on Four Group Partitioning Process Developed in JAERI, Proc. of Global ’97,1997.vol.1: 458

[43] Ozawa M, Koma Y, Nomura K, Tanaka Y. J. Alloy. Compounds, 1998,271/273:538-543

[44] Koma Y, Watanabe M, Nemoto S, Tanaka Y.Solvent Extr. Ion Exch., 1998,16 (6):1357-1367

[45] Japan Atomic Energy Agency, The Japan Atomic Power Company. Feasibility Study on Commercialized Fast Reactor Cycle System (Phase II), Final Report, March 2006 (in Japanese)

[46] Japan Science and Technology Agency, Innovative Nuclear Research and Development program-Special Promotion Area, July 2006. http://www.jst.go.jp/nrd/bosyu/h18tokushinbosyu.html (in Japanese)

[47] http://www.aec.go.jp/jicst/NC/senmon/bunri/siryo/bunri03/siryo2-2.pdf

[48] Wei Y Z, Hoshi H, Kumagai M, Asakura T, Morita Y. J. Alloys Compounds, 2004,374(1/2) :447-450

[49] Hoshi H, Wei Y Z, Kumagai M, Asakura T, Morita Y. J. Alloys Compounds,2004, 374(1/2) :451-455

[50] Wei Y Z, Hoshi H, Kumagai M, Asakura T, Uchiyama G. J. Nucl. Sci. Technol.,2002,Suppl. 3 : 761

[51] Wei Y Z, Hoshi H, Morita Y, Bruggeman A, Goethals P. Separation of Am and Cm from HLLW by Extraction Chromatography Using Novel R-BTP Extraction Resins, Proceedings of Global’2009,Paris,2009. 9390

[52] Adnet J M, Donnet L, Chartier D, Bros P, Fire N, Brossard P. The Development of the SESAME Process, Proc. of Global ’97, 1997.vol.1:592

[53] Suzuki T, Takahashi K, Nogami M, Nomura M, Ozawa M, Koyama S, Mimura H, Fujita R, Fujii Y. Concept of Advanced Spent Fuel Reprocessing based on Ion Exchange, GLOBAL 2007, USA. 2007

[54] Kubota M. Radiochimica Acta,1993,63:91-96

[55] Kubota M, Yamaguchi I, Morita Y, Yamagishi I. Radiochemistry,1997 39:299-303

[56] Paviet-Hartmann P, Raymond A. Separation of 99Tc from Real Effluents by Crown Ethers, Proc.of Global ’99, 1999

[57] Dozol J F, Lamare V, Simon N, Eymard S, Rouquette H, Tournois B. New Calix

[4] Crown for the Selective Extraction of Cesium, Proc. of Global ’97, 1997,vol.2:1517

[58] Horwitz E P, Dietz M L, Fisher D E. Solvent Extr. Ion Exch.,1991,9(1):1-25

[59] Wood D J, Law J D, Herbst R S, Todd T A. Removal of Sr and Hg from Acidic Liquid Radioactive Waste by Solvent Extraction with the SREX Process, Proc. of Global ’99, 1999

[60] Inoue M, et al., Development of Pyropartitioning of Transuranium Elements from High-Level Liquid Waste、CRIEPI Research Report, 1998. T57 (in Japanese)

[61] Kurata M, Kinoshita K, Hijikata T, Inoue T. J. Nucl. Sci. Technol.,2000,37(8):682-690

[62] Uozumi K, Kinoshita K, Inoue T, Fusselman S P, Grimmett D L, Roy J J, Storvick T S, Krueger C L, Nabelek C R. J. Nucl. Sci.Technol.,2001,38(1):36-44

[63] Kinoshita K, Kurata M, Inoue T. J. Nucl.Sci.Techmol.,2000,37(1):75-83

[64] Iizuka M, Uozumi K, Inoue T, Iwai T, Shirai O, Arai Y. J. Nucl. Mater.,2001,299:32-42

[65] Ahn D H. Development of the Electrowinning System for TRU Recovery in Korea, The 9th Joint Workshop between China and Korea on Nuclear Waste Management and Nuclear Fuel Cycle, 2010,China

[66] Harman K M, Jansen G Jr. The salt cycle process, Progress in Nuclear Energy Series III, Process Chemistry, 1970,vol.4:429

[67] Bychkov A V, Vavilov S K, Porodnov P T, Skiba O V. Pyroelectrochemical Reprocessing of Irradiated Uranium-plutonium Oxide Fuel for Fast Reactors, Proc. of Global ’93, 1993,vol.2: 1351

[68] Ivanov V B, Mayorshin A A, Skiba O V. et a1.The Utilization of Plutonium in Nuclear Reactors on the Bases of Technologies,Developed in SSC RIAR, Proc.of Global ’97,1997,vol2: 1093

[69] Suzuki K,Namba T,Asou M,et a1. Feasibility Study of Pyrochemieal Recovery of Actinide from MOX Fuel, Proc.of Global’95,1995,vol2:1200

[70] Asou M,Hasuike T,Tamura S,et a1. A Modular Recycling Plant Concept, Flexible to Future Fuel Cycle Demands, Proc. of Global ’97, 1997,vol.2:894

[71] Aso M, Mizuguchi K, Shoji Y, Kobayashi T. Theoretical Evaluation of Decontamination Methods for Noble Metals in Oxide Electrowinning Process,Proc.of Global 2001, 2001

[72] Kani Y, Sasahira A, Hoshino K, Kawamura F. Journal of Fluorine Chemistry, 2009, 130(1):74-82

[73] Akai Y, Fujita R. J. Nucl. Sci. Technol., 1995, 33:1064-1066
[1] Ye Guoan, Zhang Hu. A Review on the Development of Spent Nuclear Fuel Reprocessing and Its Related Radiochemistry [J]. Progress in Chemistry, 2011, 23(7): 1289-1294.
[2] Zhu Liyang, Wen Mingfen, Duan Wuhua, Xu Jingming, Zhu Yongjun. Application of Supercritical Fluid Extraction in Reprocessing of Spent Nuclear Fuel [J]. Progress in Chemistry, 2011, 23(7): 1308-1315.
[3] Zhang Anyun, Xiao Chengliang, Chai Zhifang. Development of Silica-Based Supramolecular Recognition Materials in Reprocessing of Nuclear Spent Fuel [J]. Progress in Chemistry, 2011, 23(7): 1355-1365.
[4] Daqing Cui. A Review of Beneficial Effects of Ruducing Environment at the Near-field of KBS-3 Repository [J]. Progress in Chemistry, 2011, 23(7): 1411-1428.
[5] Yang Tongzai, Wang Xiaolin. Current Status and Prospect of Radioanalytical Chemistry in the National Defense [J]. Progress in Chemistry, 2011, 23(7): 1520-1526.