分析化学2025，Vol.53Issue(3)：397-406,10.DOI:10.19756/j.issn.0253-3820.241480
土壤中238Pu、239Pu、240Pu和241Pu的同步分离和电感耦合等离子体串联质谱分析
Determination of 238Pu,239Pu,240Pu and 241Pu in Soil by Tandem Quadrupole Inductively Coupled Plasmon-Mass Spectrometry
摘要
Abstract
Plutonium isotopes(238Pu,239Pu,240Pu and 241Pu)in the environment are important"fingerprint"nuclides in the study of nuclear activity traceability.The content of plutonium isotopes in the environmental metrics is usually very low,and the measurement of these isotopes,especially 238Pu,using mass spectrometry is seriously interfered with by the coexisting 238U.The analysis of several plutonium isotopes in soil usually requires combination of multiple measurement techniques,which leads to a long analysis time and large uncertainty in the isotope ratio.In this work,the hydrous titanium oxide(HTiO)precipitated by the hydrolysis of titanium oxydichloride(TiOCl2)under near-neutral condition was used to preconcentrate plutonium from the soil digestion solution,and the highly efficient decontamination of 238U in the sample was achieved by TK200 resin column chromatography with a decontamination factor of 108.Simulation resuts of density functional theory(DFT)showed that NH3 was considered as a promising reaction gas to eliminate the interference of 238U from 238Pu measurement using mass spectrometry due to the significant discrepancy of the chemical reactivity of U+and Pu+with the reactive gas NH3.Experiments confirmed that by optimizing the flow rates of collision gas(He)and reaction gas(NH3),the interference of 238U could be effectively suppressed,and the decontamination factor of 238U was 104.Combined with chemical separation,the overall decontamination factor of 238U could reach 1012 by using the developed method.By combining chemical separation and tandem quadrupole inductively coupled plasmon-mass spectrometry(ICP-MS/MS)measurement,the simultaneous determination of four ultra-trace plutonium isotopes in soil was realized,and the detection limit of plutonium isotopes was at the femtogram level.Analysis of the international standard reference materials(NIST-SRM-4357 and IAEA-384)showed that the established method could be successfully used for the accurate analysis of ultra-trace four plutonium isotopes(238Pu,239Pu,240Pu and 241Pu)in soil samples.关键词
钚同位素/电感耦合等离子体串联质谱/He-NH3/TK200树脂/土壤Key words
Plutonium/Tandem quadrupole inductively coupled plasmon-mass spectrometry/He-NH3/TK200 resin/Soil引用本文复制引用
郭毅超,彭晨阳,杜心雨,张峰,周浩林,史克亮,邢闪,侯小琳..土壤中238Pu、239Pu、240Pu和241Pu的同步分离和电感耦合等离子体串联质谱分析[J].分析化学,2025,53(3):397-406,10.基金项目
国家自然科学基金项目(No.12175201)、兰州大学学生创新创业行动计划项目和国民核生化灾害防护国家重点实验室开放基金项目(No.SKLNBC2024-07)资助. Supported by the National Natural Science Foundation of China(No.12175201),the Undergraduate Innovation and Entrepreneurship Training Program of Lanzhou University,and the Opening Fund of State Key Laboratory of NBC Protection for Civilian(No.SKLNBC2024-07). （No.12175201）
