人工放射性核素236U的分析方法进展及其应用

doi:10.6023/A21020074

化学学报 ›› 2021, Vol. 79 ›› Issue (6): 716-728.DOI: 10.6023/A21020074 上一篇下一篇

综述

人工放射性核素²³⁶U的分析方法进展及其应用

邵阳^a^,^*(), 杨国胜^b, 张继龙^c, 罗敏^a, 马玲玲^a, 徐殿斗^a

a 中国科学院高能物理研究所北京市射线成像技术与装备工程技术研究中心北京 100049
b 国立研究开发法人量子科学技术研究开发机构日本千叶市 2633-8555
c 国家核安保技术中心北京 102401

投稿日期:2021-02-26 发布日期:2021-04-25
通讯作者: 邵阳

作者简介:

邵阳, 助理研究员. 2019年毕业于中国科学院高能物理研究所, 获博士学位. 2018年以博士生身份在日本弘前大学辐射医疗综合研究所山田正俊课题组访问和学习一年. 主要研究方向为关键放射性核素分析方法开发与示踪应用研究.

杨国胜, 日本量子科学技术研究开发机构, 主任研究员. 主要从事环境和人体中痕量人工放射性核素的分析方法开发、示踪及剂量评估等研究(¹³⁷Cs、Te、²²⁶Ra、²³⁶U、²³⁷Np、²³⁹Pu、²⁴⁰Pu、¹²⁹I等).

基金资助:
中国科学院重点部署项目(ZDRW-CN-2018-1); 国家自然科学基金(11875266); 国家自然科学基金(U1832212); 国家自然科学基金(U1932103); 中国科学院高能物理研究所谢家麟基金(E0546BU20B)

Progress and Application on the Analysis of Anthropogenic Radionuclide ²³⁶U

Yang Shao^a(), Guosheng Yang^b, Jilong Zhang^c, Min Luo^a, Lingling Ma^a, Diandou Xu^a

a Beijing Engineering Research Center of Radiographic Techniques and Equipment, Institute of High Energy Physics, Chinese Academy of Sciences, Beijing 100049, China
b National Institutes for Quantum and Radiological Science and Technology, Chiba, 263-8555, Japan
c State Nuclear Security Technology Center, Beijing 102401, China

Received:2021-02-26 Published:2021-04-25
Contact: Yang Shao
Supported by:
Key Deployment Projects of Chinese Academy of Sciences(ZDRW-CN-2018-1); National Natural Science Foundation of China(11875266); National Natural Science Foundation of China(U1832212); National Natural Science Foundation of China(U1932103); Xie Jialin Foundation, Institute of High Energy Physics, Chinese Academy of Sciences(E0546BU20B)

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摘要/Abstract

铀-236是一种重要的人工放射性核素, 是三种天然铀同位素之外可以应用在环境示踪、核应急、核取证以及核保障中的一种铀同位素. 人工²³⁶U主要是由核燃料²³⁵U经过中子照射后吸收中子产生, 因此, 不同“年龄”阶段核燃料中的²³⁶U和其他同位素的比值(指纹特征)截然不同. 同时不同反应堆类型中相应指纹特征也不尽相同. 通过监测核燃料、可疑核材料以及环境样品中不同²³⁶U/²³⁸U、²³⁶U/²³⁵U同位素比值等指纹特征即可确认反应堆运行状况、追溯核材料来源出处, 甚至可以开展放射性核污染物在环境中的迁移模拟等问题. 铀-236属于低丰度同位素, 其在核样品和环境样品中含量极低, 因此, 精确测定其同位素比值对²³⁶U在环境示踪、核应急、核取证以及核保障中的应用尤为重要. 本综述中, 作者总结了近年来痕量²³⁶U测定时样品前处理和检测分析技术的发展, 尤其着重于²³⁶U同位素比值的质谱检测技术的发展, 以及²³⁶U在核保障和环境中的示踪应用的研究进展. 最后, 对痕量²³⁶U检测和应用方面的研究提出展望.

关键词: ²³⁶U, 质谱分析, 前处理方法, 示踪应用, 核保障

Uranium-236 is an important anthropogenic radionuclide except for the three main natural uranium isotopes, which could be applied in the fields of environmental tracer, nuclear emergency response, nuclear forensics and nuclear safeguards. Artificial ²³⁶U is mainly generated through neuron absorption of nuclear fuel ²³⁵U after neuron irradiation. Therefore, the isotopic ratios of ²³⁶U with other uranium isotopes (fingerprints) are different at different nuclear fuel age. Also, the corresponding fingerprints are different in different types of nuclear reactor. The operation statue of nuclear reactor, the source of nuclear material and the migration of released radionuclides in environment could be studied by analyzing the isotopic ratios of ²³⁶U/²³⁸U and ²³⁶U/²³⁵U in the corresponding samples. Since ²³⁶U is a minor isotope and its concentration is extremely low in nuclear material and environmental samples, it is important to accurately analyze the isotopic ratios for its application in the environmental tracer, nuclear emergency response, nuclear forensics and nuclear safeguards. In this review, we summarized the development of sample pretreatment and analysis technologies for ²³⁶U measurement in recent years, especially focused on the development of ²³⁶U isotopic ratio analysis using mass spectrometry, and the research progress of ²³⁶U application in the fields of nuclear safeguards and environmental tracer was also reviewed. The research prospect for ²³⁶U analysis and application was also proposed.

Key words: ²³⁶U, mass spectrometry, pretreatment technique, tracer application, nuclear safeguards

引用此文

邵阳, 杨国胜, 张继龙, 罗敏, 马玲玲, 徐殿斗. 人工放射性核素²³⁶U的分析方法进展及其应用[J]. 化学学报, 2021, 79(6): 716-728.

Yang Shao, Guosheng Yang, Jilong Zhang, Min Luo, Lingling Ma, Diandou Xu. Progress and Application on the Analysis of Anthropogenic Radionuclide ²³⁶U[J]. Acta Chimica Sinica, 2021, 79(6): 716-728.

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样品类型	检测核素	树脂色谱柱	铀回收率	参考文献
珊瑚	²³⁶U、^239,240Pu	AG 1-X8、UTEVA	—	[45]
海水	²³⁶U、^239,240Pu	TEVA、UTEVA	约60%	[17]
海水	²³⁶U、²³⁷Np、^239,240Pu	TEVA、UTEVA	82%~100%	[21]
水样	^238,239,240Pu、²³⁷Np、^228,232Th、^{234,235,236,238}U、²⁴¹Am、^242,243,244Cm、¹⁴⁷Pm、⁹⁰Y、^89,90Sr、⁵⁵Fe	AG MP-1M、UTEVA、DGA、Sr、TRU	100%	[46]
水样	²³⁸U、²³²Th、²²⁶Ra、²¹⁰Po、²¹⁰Pb	TRU、Sr、HRa	93%±7%	[47]
环境擦拭样品	^{234,235,236,238}U、^{239,240,241,242}Pu	TEVA、UTEVA	>99%	[48]
土壤	^234,235,238U、^228,230,232Th	Microthene-TOPO	79.8%±13.0%	[49]
土壤	^235,238U、^239,240,241Pu	UTEVA、DOWEX^TM 1×8	—	[50]
河水	^{234,235,236,238}U、^230,232Th、^239,240Pu、²³⁷Np、²⁴¹Am、⁹⁰Sr	TEVA、DGA	93%±6.2%	[51]
海水	⁹⁹Tc、²³⁷Np、^239,240Pu、²³⁸U	TEVA、AG MP-1M、UTEVA	65%	[52]
海水	²³⁶U、²³⁷Np、^239,240Pu	TEVA、UTEVA	72.7%~112.1%	[41]

样品类型	检测核素	树脂色谱柱	铀回收率	参考文献
珊瑚	²³⁶U、^239,240Pu	AG 1-X8、UTEVA	—	[45]
海水	²³⁶U、^239,240Pu	TEVA、UTEVA	约60%	[17]
海水	²³⁶U、²³⁷Np、^239,240Pu	TEVA、UTEVA	82%~100%	[21]
水样	^238,239,240Pu、²³⁷Np、^228,232Th、^{234,235,236,238}U、²⁴¹Am、^242,243,244Cm、¹⁴⁷Pm、⁹⁰Y、^89,90Sr、⁵⁵Fe	AG MP-1M、UTEVA、DGA、Sr、TRU	100%	[46]
水样	²³⁸U、²³²Th、²²⁶Ra、²¹⁰Po、²¹⁰Pb	TRU、Sr、HRa	93%±7%	[47]
环境擦拭样品	^{234,235,236,238}U、^{239,240,241,242}Pu	TEVA、UTEVA	>99%	[48]
土壤	^234,235,238U、^228,230,232Th	Microthene-TOPO	79.8%±13.0%	[49]
土壤	^235,238U、^239,240,241Pu	UTEVA、DOWEX^TM 1×8	—	[50]
河水	^{234,235,236,238}U、^230,232Th、^239,240Pu、²³⁷Np、²⁴¹Am、⁹⁰Sr	TEVA、DGA	93%±6.2%	[51]
海水	⁹⁹Tc、²³⁷Np、^239,240Pu、²³⁸U	TEVA、AG MP-1M、UTEVA	65%	[52]
海水	²³⁶U、²³⁷Np、^239,240Pu	TEVA、UTEVA	72.7%~112.1%	[41]

采样海域	采样时间	²³⁶U/²³⁸U同位素比值	²³⁶U/²³⁸U同位素比值平均值	参考文献
North Atlantic	2014	40×10^-12~2350×10^-12	(1075±345)×10^-12	[101]
Eastern Pacific Zonal Transect	2013	0.2×10^-12~727×10^-12	(179±247)×10^-12	[103]
Greenland coastal line	2012~2016	1.1×10^-9~15.5×10^-9	3.097×10^-9	[84]
coast off Japan	2013~2015	930×10^-12~1300×10^-12	(1084±163)×10^-12	[87]
North Sea	2010	1.24×10^-9~19.49×10^-9	(7.612±3.750)×10^-9	[3]
Danish Seawater	2014	5.4×10^-9~24.0×10^-9	13.40×10^-9	[102]
western equatorial Atlantic Ocean	2010	91×10^-12~3567×10^-12	(808±1369)×10^-12	[14]
North Pacific Ocean	2012	0.09×10^-10~14.1×10^-10	(3.441±4.14)×10^-10	[95]
Arctic Ocean: Barents Sea shelf	2015	1380×10^-12~3680×10^-12	1550×10^-12	[100]
Arctic Ocean: West Spitsbergen	2015	1340×10^-12~1960×10^-12	1560×10^-12	[100]
Arctic Ocean: Eurasian Basin	2015	110×10^-12~2980×10^-12	1700×10^-12	[100]
Arctic Ocean: Makarov Basin	2015	2.8×10^-12~2810×10^-12	1670×10^-12	[100]
Fram Strait	2016	367×10^-12~2902×10^-12	(1845±654)×10^-12	[104]
Mediterranean Sea	2013	710×10^-12~2220×10^-12	(1518±369)×10^-12	[97]
northwest Mediterranean Sea	—	1.4×10^-9~2.13×10^-9	(1.78±0.33)×10^-9	[98]
northern Benguela Upwelling	2014	0.22×10^-10~6.70×10^-10	(5.091±1.596)×10^-10	[70]
Irish Sea	1993	—	(2.0±0.4)×10^-6	[13]

采样海域	采样时间	²³⁶U/²³⁸U同位素比值	²³⁶U/²³⁸U同位素比值平均值	参考文献
North Atlantic	2014	40×10^-12~2350×10^-12	(1075±345)×10^-12	[101]
Eastern Pacific Zonal Transect	2013	0.2×10^-12~727×10^-12	(179±247)×10^-12	[103]
Greenland coastal line	2012~2016	1.1×10^-9~15.5×10^-9	3.097×10^-9	[84]
coast off Japan	2013~2015	930×10^-12~1300×10^-12	(1084±163)×10^-12	[87]
North Sea	2010	1.24×10^-9~19.49×10^-9	(7.612±3.750)×10^-9	[3]
Danish Seawater	2014	5.4×10^-9~24.0×10^-9	13.40×10^-9	[102]
western equatorial Atlantic Ocean	2010	91×10^-12~3567×10^-12	(808±1369)×10^-12	[14]
North Pacific Ocean	2012	0.09×10^-10~14.1×10^-10	(3.441±4.14)×10^-10	[95]
Arctic Ocean: Barents Sea shelf	2015	1380×10^-12~3680×10^-12	1550×10^-12	[100]
Arctic Ocean: West Spitsbergen	2015	1340×10^-12~1960×10^-12	1560×10^-12	[100]
Arctic Ocean: Eurasian Basin	2015	110×10^-12~2980×10^-12	1700×10^-12	[100]
Arctic Ocean: Makarov Basin	2015	2.8×10^-12~2810×10^-12	1670×10^-12	[100]
Fram Strait	2016	367×10^-12~2902×10^-12	(1845±654)×10^-12	[104]
Mediterranean Sea	2013	710×10^-12~2220×10^-12	(1518±369)×10^-12	[97]
northwest Mediterranean Sea	—	1.4×10^-9~2.13×10^-9	(1.78±0.33)×10^-9	[98]
northern Benguela Upwelling	2014	0.22×10^-10~6.70×10^-10	(5.091±1.596)×10^-10	[70]
Irish Sea	1993	—	(2.0±0.4)×10^-6	[13]

人工放射性核素²³⁶U的分析方法进展及其应用

Progress and Application on the Analysis of Anthropogenic Radionuclide ²³⁶U

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