乏燃料干法后处理中的熔盐减压蒸馏技术

付海英; 耿俊霞; 杨洋; 罗艳; 窦强; 李文新; 李晴暖

doi:10.11889/j.0253-3219.2018.hjs.41.040001

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乏燃料干法后处理中的熔盐减压蒸馏技术

综述论文 | 更新时间：2021-05-19

- 乏燃料干法后处理中的熔盐减压蒸馏技术
- Low pressure distillation technology of molten salt in spent fuel pyroprocessing field
- 核技术 2018年41卷第4期文章编号：040001
- 作者机构：
  
  1.中国科学院上海应用物理研究所嘉定园区上海 201800
  2.中国科学院钍基熔盐核能系统研究中心上海 201800
- 作者简介：
  
  [ "付海英, 女, 1973年出生, 2005年于中国科学院上海应用物理研究所获博士学位, 研究领域为乏燃料干法后处理", "FU Haiying, female, born in 1973, graduated from Shanghai Institute of Applied Physics, Chinese Academy of Sciences with a doctoral degree in 2005, focusing on the pyroprocessing technology of spent nuclear fuel" ]
  窦强, E-mail:douqiang@sinap.ac.cn DOU Qiang, E-mail: douqiang@sinap.ac.cn
- 基金信息：
  
  国家自然科学基金(NSFC21771188);国家自然科学基金(21601201);中国科学院战略性科技先导专项-钍基熔盐堆核能系统(XDA02030000);中国科学院前沿科学重点研究项目-钍铀燃料循环特性和若干关键问题研究(QYZDY-SSWJSC016)
- DOI：10.11889/j.0253-3219.2018.hjs.41.040001
  中图分类号： TL24
- 收稿日期：2017-11-21，
  
  修回日期：2018-01-02，
  
  纸质出版日期：2018-04-10
- 稿件说明：
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付海英, 耿俊霞, 杨洋, 等. 乏燃料干法后处理中的熔盐减压蒸馏技术[J]. 核技术, 2018,41(4):040001

Haiying FU, Junxia GENG, Yang YANG, et al. Low pressure distillation technology of molten salt in spent fuel pyroprocessing field[J]. Nuclear techniques, 2018, 41(4): 040001
付海英, 耿俊霞, 杨洋, 等. 乏燃料干法后处理中的熔盐减压蒸馏技术[J]. 核技术, 2018,41(4):040001 DOI： 10.11889/j.0253-3219.2018.hjs.41.040001.

Haiying FU, Junxia GENG, Yang YANG, et al. Low pressure distillation technology of molten salt in spent fuel pyroprocessing field[J]. Nuclear techniques, 2018, 41(4): 040001 DOI： 10.11889/j.0253-3219.2018.hjs.41.040001.

摘要

本文扼要介绍了熔盐减压蒸馏技术在美国橡树岭国家实验室用于熔盐反应堆氟化物熔盐回收，以及近年来美、韩、日和法等国用于水堆/快堆乏燃料中熔盐电解阴极产物纯化的概况，分析减压蒸馏技术在这两个领域应用中面临的挑战，提出可能的发展策略。进一步强调指出，蒸馏分离技术需要与放射化学相结合，形成化学反应-蒸馏/减压蒸馏的新模式，以应对钍基熔盐反应堆乏燃料干法后处理的严峻挑战。

Abstract

Low pressure distillation technology can be used to separate components of spent fuel due to their different volatility. This paper introduced the development of molten salt distillation technology briefly. First

the fluoride salts from molten salt experiment reactor (MSRE) were recovered and reused in Oak Ridge National Laboratory (ORNL) of USA. In the last decades

the distillation technology was used to purify the cathode products after the electrochemical treatment of spent fuel from pressure water reactor (PWR) or fast reactor in USA

Japan

Korea

France and so on. Then the challenges of distillation technology in both the salt recovery and cathode products purity were illustrated and development strategies were suggested. It is further pointed out that distillation separation combined with chemistry reaction may cope with the grave challenges of spent fuel pyroprocessing for thorium molten salt reactor (TMSR).

关键词

Keywords

references

Goff K M, Simpson M F. Dry processing of used nuclear fuel[C]. Proceedings of Global 2009, INL/Con-09-15984. Goff 2009. http://www.researchgate.net/publication/255210988_Dry_Processing_of_Used_Nuclear_Fuel

刘学刚 . 乏燃料干法后处理技术研究进展 . 核化学与放射化学 , 2009 . 31 35 - 44 . http://www.wanfangdata.com.cn/details/detail.do?_type=perio&id=hhxyfshx2009z1004 .

Xuegang LIU . Research on dry reprocessing technology of spent nuclear fuel . Journal of Nuclear and Radiochemistry , 2009 . 31 35 - 44 . http://www.wanfangdata.com.cn/details/detail.do?_type=perio&id=hhxyfshx2009z1004 .

Rosenthal M W, Haubenreich P N, Briggs R B. The development status of molten-salt breeder reactors[R]. ORNL-4812, USA: ORNL, 1972. http://www.osti.gov/scitech/biblio/4622532

H Lee , G I Park , W H Kang , . Pyroprocessing technology development at KAERI . Nuclear Engineering and Technology , 2011 . 43 ( 4 ): 317 - 328 . DOI: 10.5516/NET.2011.43.4.317 http://doi.org/10.5516/NET.2011.43.4.317 .

M Iizuka , M Akagi , T Koyama . High-temperature distillation and consolidation of U-Zr cathode product from molten salt electrorefining of simulated metallic fuel . Journal of Nuclear Materials , 2014 . 448 ( 1-3 ): 259 - 269 . DOI: 10.1016/j.jnucmat.2014.02.015 http://doi.org/10.1016/j.jnucmat.2014.02.015 .

R Pierce , T Caldwell , D Pak . Application of vacuum salt distillation technology for the removal of fluoride and chloride from legacy fissile materials . Separation Science and Technology , 2012 . 47 2065 - 2073 . DOI: 10.1080/01496395.2012.697508 http://doi.org/10.1080/01496395.2012.697508 .

G Bourgès , S Faure , B Fiers , . Vacuum distillation of plutonium pyrochemical salts . Procedia Chemistry , 2012 . 7 731 - 739 . DOI: 10.1016/j.proche.2012.10.111 http://doi.org/10.1016/j.proche.2012.10.111 .

Robertson R C. Conceptual design study of a single-fluid molten-salt breeder[R]. ORNL-4541, USA: ORNL, 1971. http://www.researchgate.net/publication/236483454_Conceptual_Design_Study_of_a_Single-Fluid_Molten_Salt_Breeder_Reactor

Kelly M J. Recovery of carrier salt by distillation[R]. ORNL-3789, USA: ORNL, 1965.

A J Singh , R G Ross , R E Thoma . Vacuum distillation of LiF . Journal of Applied Physics , 1964 . 36 ( 4 ): 1367 - 1370 . DOI: 10.1063/1.1714310 http://doi.org/10.1063/1.1714310 .

Scott C D, Carter W L. Distillation of molten salt[R]. ORNL-3830, USA: ORNL, 1965: 301.

Cantor S. Transpiration studies in support of the vacuum distillation process[R]. ORNL-4037, USA: ORNL, 1967: 140-142.

Hightower J, McNeese L E. Measurement of the relative volatilities of fluorides of Ce, La, Pr, Nd, Sm, Eu, Ba, Sr, Y and Zr in mixtures of LiF and BeF 2 [R]. ORNL-TM-2058, USA: ORNL, 1968. http://www.researchgate.net/publication/236515720_MEASUREMENT_OF_THE_RELATIVE_VOLATILITIES_OF_FLUORIDES_OF_Ce_La_Pr_Nd_Sm_Eu_Ba_Sr_Y_AND_Zr_IN_MIXTURES_OF_LiF_AND_BeF_

Carter W, Lindauer R, McNeese L. Design of an engineering-scale, vacuum distillation experiment for molten-salt reactor fuel[R]. ORNL-TM-2213, Oak Ridge National Laboratory, 1968. http://www.researchgate.net/publication/255481607_DESIGN_OF_AN_ENGINEERING-SCALE_VACUUM_DISTILLATION_EXPERIMENT_FOR_MOLTEN_SALT_REACTOR_FUEL

Hightower J R, McNeese L E. Low-pressure distillation of molten fluoride mixtures: nonradioactive tests for the MSRE distillation experiment[R]. ORNL-4434, 1971. http://www.researchgate.net/publication/255217665_LOW-PRESSURE_DISTILLATION_OF_MOLTEN_FLUORIDE_MIXTURES_NONRADIOACTIVE_TESTS_FOR_THE_MSRE_DISTILLATION_EXPERIMENT

Hightower J R, McNeese L E. Low pressure distillation of a portion of the fuel salt from the molten salt reactor experiment[R]. ORNL-4577, 1971. http://www.researchgate.net/publication/255217957_LOW-PRESSURE_DISTILLATION_OF_A_PORTION_OF_THE_FUEL_CARRIER_SALT_FROM_THE_MOLTEN_SALT_REACTOR_EXPERIMENT

J R Hightower , L E McNeese . Low-pressure distillation of molten mixtures of lithium fluoride, beryllium fluoride, and zirconium fluoride for removal of rare-earth fission products . Industrial and Engineering Chemistry, Process Design and Development , 1973 . 12 ( 3 ): 232 - 236 . DOI: 10.1021/i260047a004 http://doi.org/10.1021/i260047a004 .

窦强 , 付海英 , 杨洋 , . 温度与气压对LiF熔盐蒸发速率的影响 . 核化学与放射化学 , 2014 . 36 ( 6 ): 357 - 362 . DOI: 10.7538/hhx.2014.36.06.0357 http://doi.org/10.7538/hhx.2014.36.06.0357 .

Qiang DOU , Haiying FU , Yang YANG , . Distillation behaviors of LiF salt under different pressures and evaporation temperatures . Journal of Nuclear and Radiochemistry , 2014 . 36 ( 6 ): 357 - 362 . DOI: 10.7538/hhx.2014.36.06.0357 http://doi.org/10.7538/hhx.2014.36.06.0357 .

耿俊霞 , 窦强 , 王子豪 , . 钍基熔盐堆核能系统中熔盐的蒸馏纯化与分离 . 核化学与放射化学 , 2017 . 39 ( 1 ): 36 - 42 . DOI: 10.7538/hhx.2016.YX.2015081 http://doi.org/10.7538/hhx.2016.YX.2015081 .

Junxia GENG , Qiang DOU , Zihao WANG , . Purification and separation of fluoride molten salt in thorium molten salt reactors system by low pressure distillation . Journal of Nuclear and Radiochemistry , 2017 . 39 ( 1 ): 36 - 42 . DOI: 10.7538/hhx.2016.YX.2015081 http://doi.org/10.7538/hhx.2016.YX.2015081 .

贾昀澎 , 王子豪 , 耿俊霞 , . FLiNaK熔盐中CsF的蒸发行为与分离研究 . 核技术 , 2016 . 39 ( 2 ): 020602 DOI: 10.11889/j.0253-3219.2016.hjs.39.020602 http://doi.org/10.11889/j.0253-3219.2016.hjs.39.020602 http://www.j.sinap.ac.cn/hejishu/CN/abstract/abstract548.shtml .

Yunpeng JIA , Zihao WANG , Junxia GENG , . Evaporation and separation of CsF in FLiNaK molten salt . Nuclear Techniques , 2016 . 39 ( 2 ): 020602 DOI: 10.11889/j.0253-3219.2016.hjs.39.020602 http://doi.org/10.11889/j.0253-3219.2016.hjs.39.020602 http://www.j.sinap.ac.cn/hejishu/CN/abstract/abstract548.shtml .

Z H Wang , H Y Fu , Y Yang , . The evaporation behaviors of rare earth doped FLiNaK melts during low pressure distillation . Journal of Radioanalytical and Nuclear Chemistry , 2017 . 311 ( 1 ): 637 - 642 . DOI: 10.1007/s10967-016-5110-0 http://doi.org/10.1007/s10967-016-5110-0 .

B R Westphal , K C Marsden , J C Price , . On the development of a distillation process for the electrometallurgical treatment of irradiated spent nuclear fuel . Nuclear Engineering and Technology , 2008 . 40 ( 3 ): 163 - 174 . DOI: 10.5516/NET.2008.40.3.163 http://doi.org/10.5516/NET.2008.40.3.163 .

B R Westphal , K C Marsden , J C Price . Development of a ceramic-lined crucible for the separation of salt from uranium . Metallurgical and Materials Transactions A , 2009 . 40 ( 12 ): 2861 - 2866 . DOI: 10.1007/s11661-009-9957-3 http://doi.org/10.1007/s11661-009-9957-3 .

B R Westphal , J C Price , D Vaden , . Engineering-scale distillation of cadmium for actinide recovery . Journal of Alloys and Compounds , 2007 . 444-445 561 - 564 . DOI: 10.1016/j.jallcom.2007.02.072 http://doi.org/10.1016/j.jallcom.2007.02.072 .

T Kato , M Iizuka , T Inoue , . Distillation of cadmium from uranium-plutonium-cadmium alloy . Journal of Nuclear Materials , 2005 . 340 ( 2 ): 259 - 265 . DOI: 10.1016/j.jnucmat.2004.12.002 http://doi.org/10.1016/j.jnucmat.2004.12.002 .

H C Eun , H C Yang , H S Lee , . Distillation and condensation of LiCl-KCl eutectic salts for a separation of pure salts from salt wastes from an electrorefining process . Journal of Nuclear Materials , 2009 . 395 ( 1-3 ): 58 - 61 . DOI: 10.1016/j.jnucmat.2009.09.016 http://doi.org/10.1016/j.jnucmat.2009.09.016 .

H C Yang , H C Eun , I T Kim . Study on the distillation rates of LiCl-KCl eutectic salt under different vacuum conditions . Vacuum , 2010 . 84 751 - 755 . DOI: 10.1016/j.vacuum.2009.06.011 http://doi.org/10.1016/j.vacuum.2009.06.011 .

K M Park , S W Kwon , S B Park , . The evaporation characteristics of LiCl-KCl eutectic salt from uranium deposits using batch type vacuum distiller with temperature slope of each zones . Journal of Radioanalytical and Nuclear Chemistry , 2012 . 293 ( 3 ): 857 - 862 . DOI: 10.1007/s10967-012-1766-2 http://doi.org/10.1007/s10967-012-1766-2 .

H C Eun , H C Yang , Y Z Cho , . Vacuum distillation of a mixture of LiCl-KCl eutectic salts and RE oxidative precipitates and a dechlorination and oxidation of RE oxychlorides . Journal of Hazardous Materials , 2008 . 160 634 - 637 . DOI: 10.1016/j.jhazmat.2008.03.079 http://doi.org/10.1016/j.jhazmat.2008.03.079 .

E Y Choi , C Y Won , D S Kang , . Production of uranium metal via electrolytic reduction of uranium oxide in molten LiCl and salt distillation . Journal of Radioanalytical and Nuclear Chemistry , 2015 . 304 ( 2 ): 535 - 546 . DOI: 10.1007/s10967-014-3842-2 http://doi.org/10.1007/s10967-014-3842-2 .

I S Kim , D Y Chung , M S Park , . Evaporation of CsCl, BaCl 2 , and SrCl 2 from the LiCl-Li 2 O molten salt of the electrolytic reduction process . Journal of Radioanalytical and Nuclear Chemistry , 2015 . 303 223 - 227 . DOI: 10.1007/s10967-014-3330-8 http://doi.org/10.1007/s10967-014-3330-8 .

S W Kwon , J Y Kim , D H Ahn , . A study on the evaporation of cadmium for the recovery of actinides from a liquid cathode . Journal of Radioanalytical and Nuclear Chemistry , 2010 . 284 ( 1 ): 143 - 149 . DOI: 10.1007/s10967-010-0446-3 http://doi.org/10.1007/s10967-010-0446-3 .

S W Kwon , K M Park , H G Ahn , . Separation of adhered salt from uranium deposits generated in electro-refiner . Journal of Radioanalytical and Nuclear Chemistry , 2011 . 288 789 - 793 . DOI: 10.1007/s10967-011-0988-z http://doi.org/10.1007/s10967-011-0988-z .

Y J Cho , H C Yang , H C Eun , . Oxidation of lanthanum chloride in a LiCl-KCl eutectic molten salt using the oxygen sparging method . Journal of Industrial & Engineering Chemistry , 2005 . 11 ( 5 ): 707 - 711 . http://www.researchgate.net/publication/288777768_Oxidation_of_lanthanum_chloride_in_a_LiCl-KCl_eutectic_molten_salt_using_the_oxygen_gas_sparging_method .

V A Volkovich , T R Griffiths , R C Thied . Treatment of molten salt wastes by phosphate precipitation:removal of fission product elements after pyrochemical reprocessing of spent nuclear fuels in chloride melts . Journal of Nuclear Materials , 2003 . 323 49 - 56 . DOI: 10.1016/j.jnucmat.2003.08.024 http://doi.org/10.1016/j.jnucmat.2003.08.024 .

H C Eun , Y Z Cho , H S Park , . Study on a recovery of rare earth oxides from a LiCl-KCl-RECl 3 system . Journal of Nuclear Materials , 2011 . 408 110 - 115 . DOI: 10.1016/j.jnucmat.2010.11.021 http://doi.org/10.1016/j.jnucmat.2010.11.021 .

H C Eun , J H Choi , N Y Kim , . A reactive distillation process for the treatment of LiCl-KCl eutectic waste salt containing rare earth chlorides . Journal of Nuclear Materials , 2016 . 480 69 - 74 . DOI: 10.1016/j.jnucmat.2016.07.063 http://doi.org/10.1016/j.jnucmat.2016.07.063 .

江绵恒 , 徐洪杰 , 戴志敏 . 未来先进核裂变能——TMSR核能系统 . 中国科学院院刊 , 2012 . 27 ( 3 ): 365 - 374 . DOI: 10.3969/j.issn.1000-3045.2012.03.016 http://doi.org/10.3969/j.issn.1000-3045.2012.03.016 .

Mianheng JIANG , Hongjie XU , Zhimin DAI . Advanced fission energy program-TMSR nuclear energy system . Bulletin of Chinese Academy of Sciences , 2012 . 27 ( 3 ): 365 - 374 . DOI: 10.3969/j.issn.1000-3045.2012.03.016 http://doi.org/10.3969/j.issn.1000-3045.2012.03.016 .

L Stein . Protactinium fluorides . Inorganic Chemistry , 1964 . 3 ( 7 ): 995 - 998 . DOI: 10.1021/ic50017a016 http://doi.org/10.1021/ic50017a016 .

The WPFC Expert Group. Spent nuclear fuel reprocessing flowsheet[R]. Nuclear Science NEA/NSC/WPFC/DOC (2012)15.

Majumdar D, Jahshan S N, Allison C M, et al . Recycling of nuclear spent fuel with AIROX processing: DOE/ID-10423[R]. US: DOE, 1992. http://www.researchgate.net/publication/236450005_Recycling_of_nuclear_spent_fuel_with_AIROX_processing

李文新 , 李晴暖 . 熔盐反应堆——放射化学创新发展的新源泉 . 核化学与放射化学 , 2016 . 38 ( 6 ): 326 - 336 . DOI: 10.7538/hhx.2016.38.06.0327 http://doi.org/10.7538/hhx.2016.38.06.0327 .

Wenxin LI , Qingnuan LI . Molten salt reactor:a new source of innovation development for radiochemistry . Journal of Nuclear and Radiochemistry , 2016 . 38 ( 6 ): 326 - 336 . DOI: 10.7538/hhx.2016.38.06.0327 http://doi.org/10.7538/hhx.2016.38.06.0327 .

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