电感耦合等离子体质谱法快速准确表征浓缩铀材料

O657.63; 本研究联合三重四极杆电感耦合等离子体质谱(ICP-QQQ-MS)和多接收电感耦合等离子体质谱(MC-ICP-MS),快速准确地测量浓缩铀材料中铀同位素丰度比值、230Th/234U和231Pa/235U原子物质的量比值,并诊断铀年龄.结果表明,Neptune XT型MC-ICP-MS和Agilent 8800型ICP-QQQ-MS对233U丰度的有效检测限分别为3×10-9和6 × 10-10,适用于233U丰度高于6 × 10-8和样品量充足的样品,对10-7量级233 U/235 U同位素丰度比的测量精密度达到1.0%(2a)和4.8%(2a).采用GBW04240作为外...

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Published in质谱学报 Vol. 44; no. 6; pp. 797 - 806
Main Authors 汪伟, 徐江, 席瑞阳, 王亚龙, 郭思琪, 方随, 李志明, 林剑锋, 张海涛, 张小林, 王春杰, 何亚姣
Format Journal Article
LanguageChinese
Published 西北核技术研究所,陕西西安 710024 01.11.2023
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ISSN1004-2997
DOI10.7538/zpxb.2023.0046

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Abstract O657.63; 本研究联合三重四极杆电感耦合等离子体质谱(ICP-QQQ-MS)和多接收电感耦合等离子体质谱(MC-ICP-MS),快速准确地测量浓缩铀材料中铀同位素丰度比值、230Th/234U和231Pa/235U原子物质的量比值,并诊断铀年龄.结果表明,Neptune XT型MC-ICP-MS和Agilent 8800型ICP-QQQ-MS对233U丰度的有效检测限分别为3×10-9和6 × 10-10,适用于233U丰度高于6 × 10-8和样品量充足的样品,对10-7量级233 U/235 U同位素丰度比的测量精密度达到1.0%(2a)和4.8%(2a).采用GBW04240作为外标校正质量分馏效应,建立了基于ICP-QQQ-MS的10-5量级原子物质的量比值的230Th/234U和10-8量级原子物质的量比值的231 Pa/235U的同时测量方法,对230Th-234U和231Pa-235U模式年龄的检测限分别达到 0.2 a 和 0.5 a,定年不确定度为 0.65 a(2σ)和 0.67 a(2σ).结合 MC-ICP-MS 测量的 234 U/235 U、235 U/238 U和236U/235U等同位素丰度比值,判断某批次浓缩铀样品可能用于实验堆,最后一次分离纯化时间在2009年左右,且均已经历反应堆辐照.该技术将铀年龄诊断由经典系统分离定量方法的1个月左右缩短至1周以内,分析速度快、结果准确,可为核取证、核标准物质研制定值和核保障监督等提供技术支持.
AbstractList O657.63; 本研究联合三重四极杆电感耦合等离子体质谱(ICP-QQQ-MS)和多接收电感耦合等离子体质谱(MC-ICP-MS),快速准确地测量浓缩铀材料中铀同位素丰度比值、230Th/234U和231Pa/235U原子物质的量比值,并诊断铀年龄.结果表明,Neptune XT型MC-ICP-MS和Agilent 8800型ICP-QQQ-MS对233U丰度的有效检测限分别为3×10-9和6 × 10-10,适用于233U丰度高于6 × 10-8和样品量充足的样品,对10-7量级233 U/235 U同位素丰度比的测量精密度达到1.0%(2a)和4.8%(2a).采用GBW04240作为外标校正质量分馏效应,建立了基于ICP-QQQ-MS的10-5量级原子物质的量比值的230Th/234U和10-8量级原子物质的量比值的231 Pa/235U的同时测量方法,对230Th-234U和231Pa-235U模式年龄的检测限分别达到 0.2 a 和 0.5 a,定年不确定度为 0.65 a(2σ)和 0.67 a(2σ).结合 MC-ICP-MS 测量的 234 U/235 U、235 U/238 U和236U/235U等同位素丰度比值,判断某批次浓缩铀样品可能用于实验堆,最后一次分离纯化时间在2009年左右,且均已经历反应堆辐照.该技术将铀年龄诊断由经典系统分离定量方法的1个月左右缩短至1周以内,分析速度快、结果准确,可为核取证、核标准物质研制定值和核保障监督等提供技术支持.
Abstract_FL The characteristics of enriched uranium materials are very important for nuclear fuel cycle and nuclear forensic analysis.Among all those fingerprints,the urani-um isotope ratios and the uranium age are considered to be of major parameters for trac-ing the sources and process conditions.To the best of our knowledge,there are only a few relevant articles focusing on the analysis of 233 U isotope abundance.In most of the published literatures subjected to uranium age dating,either 230Th-234 U chronometer or 231 Pa-235 U chronometer was employed to determine the age of enriched uranium materials with the isotope dilution mass spectrometry and anion exchange separation procedure,where the most time-consuming step was the sample preparation.Hence,this project aimed to develop a fast and flexible method for the determination of the uranium isotope ratios,230Th/234 U and 231 Pa/235 U atom ratios of the enriched uranium samples by the combination of multiple collector inductively coupled plasma mass spectrometry(MC-ICP-MS)and triple quadrupole inductively coupled plasma mass spectrometry(ICP-QQQ-MS).The results showed that the limits of detection(LODs)of 233 U by Neptune XT MC-ICP-MS and Agilent 8800 ICP-QQQ-MS were 3 × 10-9 and 6 × 10-10,respec-tively,and the relative standard deviations(RSDs)of 233 U/235 U isotope ratios at the level of 10-7 by MC-ICP-MS and ICP-QQQ-MS were 1.0%(2a)and 4.8%(2a),respectively.The standard sample bracketing(SSB)method of ICP-QQQ-MS based on the calibration of GBW04240 reference material was established to correct the mass fractionation of 230Th/234 U and 231 Pa/235 U atom ratios simultaneously.The ages of the uranium materials were diagnosed by the two parent-daughter relations of 234 U-230 Th and 235 U-231 Pa,indicating that the LODs of age dating were 0.2 a and 0.5 a,respectively.Meanwhile,the isotope ratios of 234 U/235 U,235 U/238 U and 236 U/235 U were determined by MC-ICP-MS.The fingerprints showed that the last purification time of the enriched uranium samples were around 2009 and the samples had been irradiated by the nuclear reactor.Overall,this method can reveal precise and accurate genetic signatures within one week,providing rapid technical supports for nuclear forensics,certification of nuclear reference materials and nuclear safeguards.
Author 王亚龙
席瑞阳
徐江
郭思琪
张海涛
汪伟
张小林
王春杰
方随
李志明
何亚姣
林剑锋
AuthorAffiliation 西北核技术研究所,陕西西安 710024
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Author_FL XU Jiang
ZHANG Xiao-lin
XI Rui-yang
FANG Sui
WANG Wei
LIN Jian-feng
HE Ya-jiao
GUO Si-qi
LI Zhi-ming
WANG Chun-jie
WANG Ya-long
ZHANG Hai-tao
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DocumentTitle_FL Rapid and Accurate Characterization of Enriched Uranium Materials by Inductively Coupled Plasma Mass Spectrometry
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Keywords uranium isotope ratios
enriched uranium materials
231Pa/235U atom ratios
uranium age
铀同位素比值
铀年龄
230Th/234U atom ratios
230Th/234U原子物质的量比值
231Pa/235U原子物质的量比值
浓缩铀材料
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Title 电感耦合等离子体质谱法快速准确表征浓缩铀材料
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