氟化物对LiCl-KCl熔盐蒸馏行为的影响

doi:10.11889/j.0253-3219.2018.hjs.41.120301

Nuclear Techniques ›› 2018, Vol. 41 ›› Issue (12): 120301-120301.doi: 10.11889/j.0253-3219.2018.hjs.41.120301

• NUCLEAR CHEMISTRY, RADIOCHEMISTRY, RADIOPHARMACEUTICALS AND NUCLEAR MEDICINE • Previous Articles Next Articles

The influence of fluorides on the distillation behaviors of molten LiCl-KCl

YANG Tianhong^1,2, LUO Yan¹, FU Haiying¹, GONG Yu¹

1 Shanghai Institute of Applied Physics, Chinese Academy of Sciences, Shanghai 201800, China;
2 University of Chinese Academy of Sciences, Beijing 100049, China

Received:2018-09-20 Revised:2018-10-10 Online:2018-12-10 Published:2018-12-13
Supported by:
Supported by the Strategic Priority Program of Chinese Academy of Sciences (No.XDA02030000), the Frontier Science Key Program of Chinese Academy of Sciences (No.QYZDY-SSWJSC016), National Natural Science Foundation of China (No.21771188)

Abstract

Abstract: [Background] Recycling the chloride salt from the fission product fluoride and chloride salt mixture is important to the research and development of electrolytic separation technology for actinides and fission products fluoride. Low pressure distillation is a powerful technique, but the experimental data on the distillation behaviors of fluoride doped chloride salts are limited.[Purpose] This study aims at the experimental results which provide a basic understanding on the behaviors of fluoride doped molten chlorides during low pressure distillation.[Methods] The distillation behaviors of various fluoride doped molten chlorides at 1050 K and 130 Pa were studied in a pipe furnace. Salt vapor was condensed and collected on stainless steel foil 5 cm away from the crucible.[Results] With the increase of evaporation ratio, the decontamination coefficient of Ce decreases at 1050 K and 130 Pa in the salt collected by 5% CeF₃-LiCl-KCl low pressure distillation. For the LiCl-KCl salts containing CeF₃, NdF₃, LaF₃ and SrF₂ respectively, the corresponding decontamination factors of the collected salts are on the order of 10³ at the evaporation ratio of 95%. The decontamination factor of EuF₃-LiCl-KCl system is very low, which may due to the presence of more volatile EuF₂ at 1050 K, while the high vapor pressure of ZrF₄is responsible for the low decontamination factor of zirconium in the case of ZrF₄-LiCl-KCl.[Conclusion] The distillation behaviors of LiCl-KCl are affected by the nature of fission product fluorides as well as the evaporation ratio of the salt mixtures. The collected chloride salt mixture from low pressure distillation of CeF₃-LiCl-KCl has a similar composition with the LiCl-KCl eutectic, and the content of fluoride is low enough.

Key words: Low pressure distillation, LiCl-KCl, Fluoride, Fission product, Decontamination factor

CLC Number:

TL426

YANG Tianhong, LUO Yan, FU Haiying, GONG Yu. The influence of fluorides on the distillation behaviors of molten LiCl-KCl[J].Nuclear Techniques, 2018, 41(12): 120301-120301.

References

1 Goff K M, Simpson M F. Dry processing of used nuclear fuel[C]. Proceedings of Global 2009, INL/Con-09-15984, 2009.
2 刘学刚. 乏燃料干法后处理技术研究进展[J]. 核化学与放射化学, 2009, 31(s1):35-44. LIU Xuegang. Research on dry reprocessing technology of spent nuclear fuel[J]. Journal of Nuclear and Radiochemistry, 2009, 31(s1):35-44.
3 Rosenthal M W, Haubenreich P N, Briggs R B. The development status of molten-salt breeder reactors[R]. ORNL-4812, USA:ORNL, 1972.
4 Kelly M J. Recovery of carrier salt by distillation[R]. ORNL-3789, USA:ORNL, 1965.
5 Singh A J, Ross R G, Thoma R E. Vacuum distillation of LiF[J]. Journal of Applied Physics, 1964, 36(4):1367-1370. DOI:10.1063/1.1714310.
6 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 BeF₂[R]. ORNL-TM-2058, USA:ORNL, 1968.
7 Cantor S. Transpiration studies in support of the vacuum distillation process[R]. ORNL-4037, USA:ORNL, 1967:140-142.
8 Scott C D, Carter W L. Preliminary design study of a continuous fluorination-vacuum distillation system for regenerating fuel and fertile streams in a molten salt breeder reactor[R]. ORNL-3791, Tennessee, USA:Oak Ridge National Laboratory, 1966.
9 Lacquement J, Bourg S, Boussier H, et al. Pyro-chemistry assessment at CEA-last experimental results[C/CD]. Proceedings of Global 2007, Boise, Idaho, 2007.
10 Lee H, Park G, Kang K, et al. Pyroprocessing technology development at KAERI[J]. Nuclear Engineering & Technology, 2011, 43(4):317-328. DOI:10.5516/NET. 2011.43.4.317.
11 Eun H C, Cho Y Z, Park H S, et al. Study on a recovery of rare earth oxides from a LiCl-KCl-RECl₃ system[J]. Journal of Nuclear Materials, 2011, 408:110-115. DOI:10.1016/j.jnucmat.2010.11.021.
12 Kim I S, Chung D Y, Park M S, et al. Evaporation of CsCl, BaCl₂, and SrCl₂ from the LiCl-Li₂O molten salt of the electrolytic reduction process[J]. Journal of Radioanalytical and Nuclear Chemistry, 2014, 303:223-227. DOI:10.1007/s10967-014-3330-8.
13 Cho Y Z, Lee T K, Eun H C, et al. Purification of used eutectic (LiCl-KCl) salt electrolyte from pyroprocessing[J]. Journal of Nuclear Materials, 2013, 437(1-3):47-54. DOI:10.1016/j.jnucmat.2013.01.344.
14 Eun H C, Choi J H, Kim N Y, et al. A reactive distillation process for the treatment of LiCl-KCl eutectic waste salt containing rare earth chlorides[J]. Journal of Nuclear Materials, 2016, 480:69-74. DOI:10.1016/j.jnucmat. 2016.07.063.
15 Wang X B, Huang W, Gong Y, et al. Electrochemical behavior of Th(IV) and its electrodeposition from ThF₄ -LiCl-KCl melt[J]. Electrochimica Acta, 2016, 196:286-293. DOI:10.1016/j.electacta.2016.02.184.
16 徐千惠, 朱铁建, 郑海洋, 等. ThF₄-LiCl-KCl熔盐体系中F^-浓度对Th(Ⅳ)电解提取的影响[J]. 辐射研究与辐射工艺学报, 2018, 36(3):030301. DOI:10.11889/j.1000-3436.2018.rrj.36.030301. XU Qianhui, ZHU Tiejian, ZHENG Haiyang, et al. Effect of F^-concentration on the electrolysis of Th(IV) in ThF₄-LiCl-KCl[J]. Journal of Radiation Research and Radiation Processing, 2018, 36(3):030301. DOI:10.11889/j.1000-3436.2018.rrj.36.030301.
17 贾昀澎, 王子豪, 耿俊霞, 等. FLiNaK熔盐中CsF的蒸发与分离[J]. 核技术, 2016, 39(2):020602. DOI:10.11889/j.0253-3219.2016.hjs.39.020602. JIA Yunpeng, WANG Zihao, GENG Junxia, et al. Evaporation and separation of CsF in FLiNaK molten salt[J]. Nuclear Techniques, 2016, 39(2):020602. DOI:10.11889/j.0253-3219.2016.hjs.39.020602.
18 Yang H C, Eun H C, Kim I T. Study on the distillation rates of LiCl-KCl eutectic salt under different vacuum conditions[J]. Vacuum, 2009, 84:751-755. DOI:10.1016/j.vacuum.2009.06.011.
19 Wang Z H, Fu H Y, Yang Y, et al. The evaporation behaviors of rare earth doped FLiNaK melts during low pressure distillation[J]. Journal of Radioanalytical and Nuclear Chemistry, 2017, 311(1):637-642. DOI:10.1007/s10967-016-5110-0.
20 Yaws C L. Handbook of vapor pressure:inorganic compounds and elements[M]. Gulf Professional Publishing, 1995, Vol 4.
21 Eun H C, Yang H C, Cho Y Z, et al. Vacuum distillation of a mixture of LiCl-KCl eutectic salts and RE oxidative precipitates and a dechlorination and oxidation of RE oxychlorides[J]. Journal of Hazardous Materials, 2008, 160:634-637. DOI:10.1016/j.jhazmat.2008.03.079.
22 Katayama Y. Precipitation of rare earth compounds in LiCl-KCl eutectic[J]. Journal of the Electrochemical Society, 1995, 142(7):2174-2178. DOI: 10.1149/1. 2044271.

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The influence of fluorides on the distillation behaviors of molten LiCl-KCl

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