激光剥蚀-多接收电感耦合等离子体质谱法测定含钚颗粒物中<sup>240</sup>Pu/<sup>239</sup>Pu比值

引用本文: 汪伟, 李志明, 徐江, 周国庆, 粟永阳, 吴艳敏, 韦冠一, 方随, 王文亮. 激光剥蚀-多接收电感耦合等离子体质谱法测定含钚颗粒物中²⁴⁰Pu/²³⁹Pu比值[J]. 分析化学, 2017, 45(11): 1719-1726. doi: 10.11895/j.issn.0253-3820.171028 shu

Citation: WANG Wei, LI Zhi-Ming, XU Jiang, ZHOU Guo-Qing, SU Yong-Yang, WU Yan-Min, WEI Guan-Yi, FANG Sui, WANG Wen-Liang. Determination of ²⁴⁰Pu/²³⁹Pu in Plutonium-containing Particle by Laser Ablation Multiple Collector Inductively Coupled Plasma Mass Spectrometry[J]. Chinese Journal of Analytical Chemistry, 2017, 45(11): 1719-1726. doi: 10.11895/j.issn.0253-3820.171028 shu

激光剥蚀-多接收电感耦合等离子体质谱法测定含钚颗粒物中²⁴⁰Pu/²³⁹Pu比值

西北核技术研究所, 西安 710024
基金项目:
本文系科技部重大仪器专项资助项目（No.2012YQ250003）

摘要: 为高精度、准确地获取含钚颗粒物中具有核保障监督意义和核取证价值的钚同位素比值，建立了激光剥蚀-多接收电感耦合等离子体质谱（LA-MC-ICP-MS）测定含钚颗粒物中²⁴⁰Pu/²³⁹Pu的分析方法。采用检漏、安装排风罩和擦拭剥蚀池内壁等方式有效降低激光剥蚀产物沾污实验室和危及人身安全的潜在风险。联用扫描电迁移率粒径谱仪（SMPS）与激光剥蚀-多接收器等离子体质谱（LA-MC-ICP-MS）研究了激光剥蚀玻璃基体标样产生气溶胶的分布特性，结果表明，剥蚀产物的主要粒径是40~500 nm，应尽量采用水平管道连接激光剥蚀进样系统与MC-ICP-MS，含钚颗粒物分析后剥蚀池持续吹扫时间应大于15 min。采用外标归一化法离线校正质量分馏效应和离子计数器检测效率，建立了含钚颗粒物中²⁴⁰Pu/²³⁹Pu的LA-MC-ICP-MS分析方法，固定束斑直径30μm、脉冲重复率5 Hz、剥蚀时间5 s，调节能量密度使含钚颗粒物模拟样品中²³⁹Pu的信号强度分别达2×10⁴cps和2×10⁵cps，本方法对²⁴⁰Pu/²³⁹Pu测量的相对实验标准不确定度小于1.4%（n=6），测量结果与参考值的相对偏差小于4.7%，仪器调试时间和单个样品测量时间分别为9.0和0.5 h。含钚颗粒物模拟样品分析结果表明，本方法精度高、结果准确、分析速度快，可满足核保障监督、禁产核查和核取证中含钚颗粒物直接分析的需求。

关键词:

English

Determination of ²⁴⁰Pu/²³⁹Pu in Plutonium-containing Particle by Laser Ablation Multiple Collector Inductively Coupled Plasma Mass Spectrometry

Northwest Institute of Nuclear Technology, Xi'an 710024, China
Received Date: 22 June 2017
Revised Date: 10 September 2017
Fund Project:
This work was supproted by the National key Foundation for Exploring Scientific Instrumet of China (No. 2012YQ250003)

Abstract: The isotopic fingerprints of plutonium are extremely important for nuclear safeguards and nuclear forensics. An analytical method was developed for direct determination of ²⁴⁰Pu/²³⁹Pu ratio in plutonium-containing particles by laser ablation multiple collector inductively coupled plasma mass spectrometry (LA-MC-ICP-MS). The risk of ablated particles leakage was reduced by leak detection, exhaust hood, and swiping the laser cell. Scanning mobility particle sizer (SMPS) was used to measure the effect of ablation parameters on the size distribution of ablated particles. The results showed that the majority of ablation material presented as particles from 40-500 nm and the sweep time after laser ablation should be longer than 15 min. The particle size was evaluated to guide LA-MC-ICP-MS system. By using external normalization method for correction of the mass fractionation correction factor and ion counter efficiencies measured by nebulizer-coupled MC-ICP-MS, a LA-MC-ICP-MS method was established for analysis of ²³⁹Pu/²⁴⁰Pu ratio in plutonium particles. Spot size, ablation rate and laser dwell time were set at 30 μm, 5 Hz and 5 s, respectively. Laser energy density was controlled to ensure that the intensities of ²³⁹Pu for plutonium-containing particles were about 2×10⁴ cps and 2×10⁵ cps, respectively. The analytical results showed that the relative uncertainties for ²³⁹Pu/²⁴⁰Pu was less than 1.4% (n=6), and the measured value deviated by less than 4.7% from the reference value. The time for adjusting system and determining ²³⁹Pu/²⁴⁰Pu ratio in single plutonium particle was 9 h and 0.5 h, respectively. The results demonstrated that this technique was rapid, precise and accurate, and could be used for determination of ²³⁹Pu/²⁴⁰Pu in plutonium-containing particles.

Key words:

Plutonium particles
/ ²⁴⁰Pu/²³⁹Pu ratio
/ Laser ablation multiple collector inductively coupled plasma mass spectrometry

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沈阳化工大学材料科学与工程学院沈阳 110142

激光剥蚀-多接收电感耦合等离子体质谱法测定含钚颗粒物中²⁴⁰Pu/²³⁹Pu比值

English

Determination of ²⁴⁰Pu/²³⁹Pu in Plutonium-containing Particle by Laser Ablation Multiple Collector Inductively Coupled Plasma Mass Spectrometry

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

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激光剥蚀-多接收电感耦合等离子体质谱法测定含钚颗粒物中240Pu/239Pu比值

English

Determination of 240Pu/239Pu in Plutonium-containing Particle by Laser Ablation Multiple Collector Inductively Coupled Plasma Mass Spectrometry

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

CCS Chemistry：静电组装导向聚合- 聚电解质纳米凝胶量化制备新策略

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

激光剥蚀-多接收电感耦合等离子体质谱法测定含钚颗粒物中²⁴⁰Pu/²³⁹Pu比值

Determination of ²⁴⁰Pu/²³⁹Pu in Plutonium-containing Particle by Laser Ablation Multiple Collector Inductively Coupled Plasma Mass Spectrometry

CCS Chemistry：颜徐州、鲍哲南：你的皮肤可能是一片SPMs