为有效获取铀颗粒物中具有取证价值的铅杂质同位素信息,建立了激光烧蚀-多接收电感耦合等离子体质谱(LA-MC-ICP-MS)测定铀颗粒物中铅杂质同位素比值的方法。探究了诸多同位素分馏效应校正方法下铅本底对同位素测量的影响,选用的LA-MC-ICP-MS系统的本底对比值测量结果的影响小于0.001(208Pb的信号强度大于2.2×103 cps),确定采用NIST SRM612为外标校正质量分馏,固定激光束斑直径30μm、脉冲重复率20 Hz、调节能量密度使LA-MC-ICP-MS分析NIST SRM612和铀颗粒物样品所得208Pb分别小于1.5×105 cps和3×104 cps,标准物质CRM124-4样品中206Pb/208Pb、206Pb/207Pb和207Pb/208Pb比值测量结果的相对实验标准不确定度小于0.48%、0.68%和0.40%。实际样品分析结果表明,本方法可有效区分铀颗粒物中的铅同位素比值差异,有助于鉴别其来源。
The isotopic abundance of lead as a signature or fingerprint in uranium has played an important role in nuclear forensics analysis. In this work, a novel analytical approach is presented to determine the isotopic abundance of lead in uranium particles by laser ablation multiple collector inductively coupled plasma mass spectrometry (LA-MC-ICP-MS). External standardization method is involved in correcting the mass fractionation in the process of analysis. The approach has been successfully validated by the measurement of CRM124-4 standard reference material. Spot size and ablation rate are set at 30 μm and 20 Hz, respectively. Laser energy density is under control to ensure that the 208Pb for NIST SRM612 and uranium particles are less than 1.5×105 cps and 3×104 cps, respectively. The results show that the relative uncertainty of 206Pb/208Pb, 206Pb/207Pb and 207Pb/208Pb ratios in CRM124-4 are less than 0.48%, 0.68% and 0.40%, respectively. Two kinds of uranium particles originated from different places have been analyzed by the proposed approach. The results demonstrate that the distinct lead isotope signatures can offer a number of evidence to determine whether the uranium particles have come directly from a mining operation or an ore-body, or whether it is anthropogenic.
参考文献
| [1] | Mayer K,Wallenius M, Lützenkirchen K, Galy J, Varga Z, Erdmann N, Buda R, Kratz J V, Trautmann N, Fifield K. Journal of Physics:Conference Series, 312,2011, 062003 |
| [2] | Mácsik Z S, Vajda N, Széles, R. Katona. IAEA-CN-184/177 |
| [3] | Donohue D. IAEA-CN-184/159 |
| [4] | XIA Yu-Liang, HAN Jun. Acta Geoscientica Sinica, 2008,29(6):752-760 夏毓亮, 韩军.地球学报,2008,29(6):752-760 |
| [5] | SHI Shao-Hua, HU Rui-Zhong, WEN Han-Jie, SUN Ru-Liang, WANG Jia, CHEN Heng. Acta Geologica Sinica, 2010,84(8):1175-1182 石少华, 胡瑞忠, 温汉捷, 孙如良, 王加, 陈恒.地质学报,2010,84(8):1175-1182 |
| [6] | FAN Chen-Zi, HU Ming-Yue, ZHAO Ling-Hao, SUN Dong-Yang, ZHAN Xiu-Chun. Rock and Mineral Analysis, 2012,31(1):29-46 范晨子, 胡明月, 赵令浩, 孙冬阳, 詹秀春.岩矿测试,2012,31(1):29-46 |
| [7] | Sylvester P J. Laser-Ablation-ICP-MS in the Earth Sciences-Principles and Applications,Translated by LIN Shou-Lin, HU Sheng-Hong, LIU Yong-Sheng, YUAN Hong-Lin, LUO Yan, Beijing:Geological Publishing House, 2003 Sylvester P J.林守麟, 胡圣虹, 刘勇胜, 袁洪林, 罗彦 译.地球科学中的激光烧蚀-ICPMS原理和应用,北京:地质出版社, 2003 |
| [8] | LIU Zhi-Min, SHI Yu-Fang, LIU Yong-Sheng, HU Zhao-Chu. Chinese J. Anal. Lab, 2010,29(4):9-13 刘智敏, 史玉芳, 刘勇胜, 胡兆初.分析试验室,2010,29(4):9-13 |
| [9] | YUAN Ji-Hai, ZHAN Xiu-Chun, HU Ming-Yue, ZHAO Ling-Hao, SUN Dong-Yang. Spectroscopy and Spectral Analysis, 2015,35(2):512-518 袁继海, 詹秀春, 胡明月, 赵令浩, 孙冬阳.光谱学与光谱分析,2015,35(2):512-518 |
| [10] | Pearce J G, Perkins W T, Westgate J A, Gorton M P, Jackson S E, Neal C R,Chenery S P. J. Geostandards Geoanal., 1997,6(21):115-144 |
| [11] | Simon J I, Reid M R, Young E D. Geochim. Cosmochim., 2007,71:2014-2035 |
| [12] | CHEN Kai-Yun, FAN Chao, YUAN Hong-Lin, BAO Zhi-An, ZONG Chun-Lei, DAI Meng-Ning, LING Xue, YANG Ying. Spectroscopy and Spectral Analysis, 2013,33(5):1342-1349 陈开运, 范超, 袁洪林, 包志安, 宗春蕾, 戴梦宁, 凌雪, 杨颖.光谱学与光谱分析,2013, 33(5):1342-1349 |
| [13] | Varga Z. Anal. Chim. Acta, 2008,625:1-7 |
| [14] | Lloyd N S, Parrish R R, Horstwood M S A, Chenery S R N. J. Anal. At. Spectrom., 2008,24:752-758 |
| [15] | WANG Wei, LI Zhi-Ming, XU Jiang, ZHOU Guo-Qing, SHEN Xiao-Pan, ZHAI Li-Hua. Chinese J. Anal. Chem., 2015,43(5):703-708 汪 伟, 李志明, 徐江, 周国庆, 沈小攀, 翟利华.分析化学,2015, 43(5):703-708 |
| [16] | Boulyga S F, Prohaska T. Anal. Bioanal. Chem., 2008, 390(2):531-539 |
| [17] | Stefánka Z, Katona R, Varga Z. J. Anal. At. Spectrom., 2008,23:1030-1033 |
| [18] | XIE Lie-Wen, YANG Jin-Hui, YANG Yue-Heng, WU Fu-Yuan. Acta Geoscientica Sinica, 2005,26:23 谢烈文, 杨进辉, 杨岳衡, 吴福元.地球学报,2005,26:23 |
| [19] | Tanimizu M, Ishikawa T. Geochem. J., 2006,40:121-133 |
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