铀材料中杂质钍的<sup>230</sup>Th/<sup>232</sup>Th比值指纹分析研究

引用本文: 徐江, 汪伟, 席瑞阳, 粟永阳, 王文亮, 李志明, 翟利华, 方随, 张海涛, 凡金龙, 王玉凤. 铀材料中杂质钍的²³⁰Th/²³²Th比值指纹分析研究[J]. 分析化学, 2022, 50(2): 310-316. doi: 10.19756/j.issn.0253-3820.210552 shu

Citation: XU Jiang, WANG Wei, XI Rui-Yang, SU Yong-Yang, WANG Wen-Liang, LI Zhi-Ming, ZHAI Li-Hua, FANG Sui, ZHANG Hai-Tao, FAN Jing-Long, WANG Yu-Feng. Fingerprinting of ²³⁰Th/²³²Th in Uranium Materials for Nuclear Forensic[J]. Chinese Journal of Analytical Chemistry, 2022, 50(2): 310-316. doi: 10.19756/j.issn.0253-3820.210552 shu

铀材料中杂质钍的²³⁰Th/²³²Th比值指纹分析研究

西北核技术研究所,西安 710024

通讯作者: 李志明,E-mail:YQ250003@nint.ac.cn

基金项目:
科技部重大仪器专项项目（No.2012YQ250003）资助

摘要: 研究了铀材料中杂质钍的²³⁰Th/²³²Th比值的核取证学属性，采用基于磷酸三丁酯(TBP)的铀钍分离流程制备低本底钍纯化液，通过铀外标校正钍的分馏效应，采用多接收电感耦合等离子体质谱(MC-ICP-MS)测定²³⁰Th/²³²Th比值。结果表明，²³⁰Th/²³²Th比值是具有时效性的铀材料特征指纹信息，流程本底引入的²³²Th浓度小于5.5×10^-11 g/g，二氧化铀芯块、黄饼YC1、平行样黄饼YC2和黄饼YC3中的²³⁰Th/²³²Th比值分别为0.479±0.037、1.376×10^-4±4.8×10^-6、2.8582×10^-3±2.2×10^-6和2.8605×10^-3±2.1×10^-6(k=2)，不确定度的主要来源是流程本底、待测样品中钍浓度，以及弱信号测量的不确定度。本方法结果准确，精密度较高，可鉴别²³⁰Th/²³²Th比值存在一定差异的铀材料，为核取证提供技术支持。

关键词:

English

Fingerprinting of ²³⁰Th/²³²Th in Uranium Materials for Nuclear Forensic

Northwest Institute of Nuclear Technology, Xi'an 710024, China

Corresponding author: LI Zhi-Ming, YQ250003@nint.ac.cn

Received Date: 08 June 2021
Revised Date: 20 November 2021
Fund Project:
Supported by the Special-Funded Program on National Key Scientific Instruments of China (No.2012YQ250003)

Abstract: Determination of thorium isotopic ratio ²³⁰Th/²³²Th in uranium materials by multiple collector inductively coupled plasma mass spectrometry (MC-ICP-MS) was presented for nuclear forensic. One piece of UO₂ formed uranium pellet and three kinds of yellow cake powder were dissolved with ultrapure HNO₃ (7.5 mol/L). Thorium was purified for analysis using a single column prepared with TBP resin bed, with which the sample was loaded and then Th was eluted with 4 mol/L HCl. Analyses were performed on Nu Plasma MC-ICP-MS and mass-bias correction were applied to the ²³⁰Th/²³²Th using bracketing measurements of U standard. An equation was proposed to correct the contribution from Th blank for calculating the ²³⁰Th/²³²Th of the uranium materials. The results showed that the ²³⁰Th/²³²Th ratios of the uranium pellet, yellow cake powder named YC1, yellow cake powder named YC2 and yellow cake powder named YC3 were (0.479±0.037), (1.376×10^-4±4.8×10^-6), (2.8582×10^-3±2.2×10^-6) and (2.8605×10^-3±2.1×10^-6) (k=2), respectively. The determined ²³⁰Th/²³²Th ratio of the uranium pellet agreed with the reference value. The yellow cake powder named YC2 and the yellow cake powder named YC3 were from the same source, whose ²³⁰Th/²³²Th ratios agreed with each other and differed distinctly from that of another sourced yellow cake powder named YC1. It was proved that the thorium isotope ratio ²³⁰Th/²³²Th was a newly discovered and time correlated fingerprint of uranium materials.

Key words:

Uranium materials
/ Fingerprint
/ ²³⁰Th/²³²Th ratio
/ Multiple collector inductively coupled plasma mass spectrometry

1. [1]
  JIANG Xiao-Yan, ZHU Liu-Chao, ZHANG Yan，ZHAO Yong-Gang, WANG Fan, WANG Tong-Xing. At. Energy Sci. Technol., 2020, 54(2): 373-378. 姜小燕, 朱留超, 张燕, 赵永刚, 王凡, 王同兴. 原子能科学技术, 2020, 54(2): 373-378.
2. [2]
  SHAO Xue-Peng, WANG Chang-Bin, TANG Lei, YANG Tian-Li, LUO Li-Li, LIU Xue-Mei, LONG Kai-Ming. Nucl. Sci. Eng., 2015, 35(4): 757-765. 邵学鹏, 王昌斌, 汤磊, 杨天丽, 罗立力, 刘雪梅, 龙开明. 核科学与工程, 2015, 35(4): 757-765.
3. [3]
  WANG Wei，FANG Sui，XU Jiang，LI Zhi-Ming，YUAN Xiang-Long，SHEN Xiao-Pan，ZHAI Li-Hua，DENG Hu，LIN Jian-Feng，KE Chang-Feng. Chin. J. Anal. Chem., 2018, 46(8): 1245-1252. 汪伟, 方随, 徐江, 李志明, 袁祥龙, 沈小攀, 翟利华, 邓虎, 林剑锋, 柯昌凤. 分析化学，2018, 46(8): 1245-1252.
4. [4]
  PARSONS-DAVIS T, KNIGHT K, FITZGERALD M, STONE G, CALDEIRA L, RAMON C, KRISTO M. Forensic Sci. Int., 2018, 286: 223-232.PARSONS-DAVIS T, KNIGHT K, FITZGERALD M, STONE G, CALDEIRA L, RAMON C, KRISTO M. Forensic Sci. Int., 2018, 286: 223-232.
5. [5]
  MADZUNYA D, UUSHONA V, MATHUTHU M, HEIKE W. J. Environ. Radioact., 2021, 237: 106668.MADZUNYA D, UUSHONA V, MATHUTHU M, HEIKE W. J. Environ. Radioact., 2021, 237: 106668.
6. [6]
  GAFFNEY A M, HUBERT A, KINMAN W S, MAGARA M, OKUBO A, POINTURIER F, SCHORZMAN K C, STEINER R E, WILLIAMS R W W. J. Radioanal. Nucl. Chem., 2016, 307: 2055-2060GAFFNEY A M, HUBERT A, KINMAN W S, MAGARA M, OKUBO A, POINTURIER F, SCHORZMAN K C, STEINER R E, WILLIAMS R W W. J. Radioanal. Nucl. Chem., 2016, 307: 2055-2060
7. [7]
  HUANG Sheng-Hui, CHANG Li, CHEN Yan, ZHAO Li-Fei, ZHU Liu-Chao, ZHAO Xing-Hong, ZHAO Yong-Gang. J. Nucl. Radiochem., 2017, 39(5): 368-372. 黄声惠, 常利, 陈彦, 赵立飞, 朱留超, 赵兴红, 赵永刚. 核化学与放射化学, 2017, 39(5): 368-372.
8. [8]
  KAYZAR-BOGGS T M, KINMAN W S, BOSTICK D A, CARDON A, FOLEY R R, HEXEL C R, KING-LOPEZ R, LINDVALL R E, MARKS N, SHARP M A, TICKNOR B W. J. Radioanal. Nucl. Chem., 2021, 327(2): 877-889.KAYZAR-BOGGS T M, KINMAN W S, BOSTICK D A, CARDON A, FOLEY R R, HEXEL C R, KING-LOPEZ R, LINDVALL R E, MARKS N, SHARP M A, TICKNOR B W. J. Radioanal. Nucl. Chem., 2021, 327(2): 877-889.
9. [9]
  WANG Qing-Quan, HU E-Ming. Uranium Extraction Technology. Harbin: Publishing House of Harbin Engineering University, 2010: 1-20. 王清泉, 胡鄂明. 铀提取工艺学. 哈尔滨: 哈尔滨工程大学出版社, 2010: 1-20.
10. [10]
  LIAO Ze-Bo, SHAO Qing-Feng, LI Chun-Hua, KONG Xing-Gong, WANG Yong-Jin. J. Chin. Mass Spectrom. Soc., 2018, 39(3): 295-309. 廖泽波, 邵庆丰, 李春华, 孔兴功, 汪永进. 质谱学报, 2018, 39(3): 295-309.
11. [11]
  LI Chun-Hua, HUANG Meng-Jie, LIAO Ze-Bo, KONG Xing-Gong, SHAO Qing-Feng. J. Chin. Mass Spectrome. Soc., 2019, 40(3): 209-221. 李春华, 黄孟杰, 廖泽波, 孔兴功, 邵庆丰. 质谱学报, 2019, 40(3): 209-221.
12. [12]
  XIE Sheng-Kai, GUO Dong-Fa, TAN Jing, ZHANG Yan-Hui, HUANG Qiu-Hong, GAO Ai-Guo. World Nucl. Geosci., 2013, 30(3): 180-186. 谢胜凯, 郭冬发, 谭靖, 张彦辉, 黄秋红, 高爱国. 世界核地质科学, 2013, 30(3): 180-186.
13. [13]
  DU Gui-Rong, GUO Guo-Long, WANG Chun-Ye, LIU Yang, SUN Xiao-Guang. J. Nucl. Radiochem., 2017,39(2): 179-182. 杜桂荣, 郭国龙, 王春叶, 刘扬, 孙晓光. 核化学与放射化学, 2017, 39(2): 179-182.
14. [14]
  ZHANG Hai-Tao, LIN Jian-Feng, XU Jiang, WANG Wei, LI Zhi-Ming. J. Nucl. Radiochem., 2020, 42(4): 235-241. 张海涛, 林剑锋, 徐江, 汪伟, 李志明. 核化学与放射化学, 2020, 42(4): 235-241.
15. [15]
  YE De-Pei. Uncertainty of Measurement. Beijing: National Defense Industry Press, 1996: 14-40. 叶德培. 测量不确定度. 北京：国防工业出版社, 1996: 14-40.

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沈阳化工大学材料科学与工程学院沈阳 110142

铀材料中杂质钍的²³⁰Th/²³²Th比值指纹分析研究

通讯作者: 李志明,E-mail:YQ250003@nint.ac.cn

English

Fingerprinting of ²³⁰Th/²³²Th in Uranium Materials for Nuclear Forensic

Corresponding author: LI Zhi-Ming, YQ250003@nint.ac.cn

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通讯作者: 陈斌, bchen63@163.com

中国化学会秘书处

铀材料中杂质钍的230Th/232Th比值指纹分析研究

通讯作者: 李志明,E-mail:YQ250003@nint.ac.cn

English

Fingerprinting of 230Th/232Th in Uranium Materials for Nuclear Forensic

Corresponding author: LI Zhi-Ming, YQ250003@nint.ac.cn

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

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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？

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通讯作者: 陈斌, bchen63@163.com

中国化学会秘书处

铀材料中杂质钍的²³⁰Th/²³²Th比值指纹分析研究

Fingerprinting of ²³⁰Th/²³²Th in Uranium Materials for Nuclear Forensic

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