基于高速示波器的多接收电感耦合等离子体质谱单颗粒分析系统的搭建及其对模拟核颗粒的同位素分析  

Development of Multiple Collector Inductively Coupled Plasma Mass Spectrometry Single Particle Analysis System Based on High-Speed Oscilloscope and Its Application to Isotopic Analysis of Individual Simulated Nuclear Particles

作　　者：邢鹏举 付媛 BELSHAW Nicholas Stanley 董俊航 刘星[1] 郑洪涛 朱振利[1,2] XING Peng-Ju;FU Yuan;BELSHAW Nicholas Stanley;DONG Jun-Hang;LIU Xing;ZHENG Hong-Tao;ZHU Zhen-Li(State Key Laboratory of Biogeology and Environmental Geology,China University of Geosciences(Wuhan),Wuhan 430070,China;Faculty of Material Science and Chemistry,China University of Geosciences(Wuhan),Wuhan 430070,China;Department of Earth Sciences,Oxford University,Oxford,OX13PR,UK)

机构地区：[1]中国地质大学(武汉),生物地质与环境地质国家重点实验室,武汉430070 [2]中国地质大学(武汉)材料与化学学院,武汉430070 [3]牛津大学地球科学系,英国牛津OX13PR

出　　处：《分析化学》2024年第10期1591-1601,共11页Chinese Journal of Analytical Chemistry

基　　金：国家自然科学基金项目(Nos.22274145,22061130207);中国载人航天工程空间应用系统和中央高校基础研究基金项目(No.G1323523047);国家重点研发计划项目(No.2022YFF0504600)资助。

摘　　要：纳米至微米级的颗粒物在环境科学、生命科学与核安全等领域受到高度关注,其元素和同位素特征分析对颗粒物溯源、评估颗粒物对人类健康和环境的潜在风险等研究具有重要意义。针对现有商品化多接收电感耦合等离子体质谱(MC-ICP-MS)检测系统存在响应速度慢、难以满足单颗粒瞬时信号分析的问题,本研究利用高速数字示波器构建了一套纳秒时间分辨的“事件触发信号捕获”(Event-triggered signal capture,ETSC)系统。将此系统与MC-ICP-MS结合,实现了稀土纳米颗粒内微小质量水平(ag~fg级别)的元素和同位素特征的准确分析。ETSC系统能够在纳秒时间分辨率下准确记录二次电子倍增器(EM)捕获的单个颗粒事件中的离子脉冲,提供单颗粒事件的完整轮廓,显著提高了单颗粒瞬时信号获取的准确度和灵敏度。结果表明,ETSC系统可以实现50 nm稀土掺杂颗粒中ag质量水平的镱(Yb)元素的定量分析,检出限低至38 ag;氧化钇模拟核颗粒的单颗粒同位素比值分析的标准偏差(SD)可达到0.047(173/171Yb),对多个氧化钇颗粒的176/171Yb和173/171Yb同位素分析的标准误差(SE)达到了2‰~3‰水平。此外,将氧化镱纳米颗粒作为模拟核颗粒添加到江水、湖水、浅层地下水和土壤等环境样品中,通过简单的颗粒提取方法,利用ETSC系统实现了颗粒同位素比值的准确分析。本研究开发的ETSC系统为单个核颗粒中ag~fg质量水平的元素与同位素分析提供了一种灵敏且具有广阔应用前景的新方法。The analysis of nano-micro nuclear particles has attracted significant attention due to the crucial role of their elemental and isotopic characteristics in tracing the origins of particulate matter and assessing its potential risks to human health and the environment.However,challenges persist in obtaining accurate and consistent element profiles and ratios for small-sized nanoparticles due to their low level and the transient nature.In this study,a high-speed digital oscilloscope was integrated with multiple collector inductively coupled plasma mass spectrometry(MC-ICP-MS)to develop a high time-resolution″Event-triggered signal capture″(ETSC)system for single particle analysis.This innovative approach enabled the analysis of element/isotope within rare earth nanoparticles at ag–fg level.The ETSC accurately recorded the complete profile of single particle,event captured by the electron multiplier with nanosecond time resolution,allowing for high-sensitivity element analysis and highprecision isotope analysis of single particles.The results demonstrated that the ETSC system could achieve quantitative analysis of ag levels of ytterbium(Yb)in 50-nm rare earth-doped particles,with a detection limit as low as 38 ag for Yb.Moreover,the isotopic precision of single particle analysis for 173/171Yb could reach 0.047(standard deviation),and the standard error for isotopic analysis of multiple particles could achieve a level of 2‰–3‰(permil)for 173/171Yb.Finally,the capability of ETSC system to analyze environmental samples was demonstrated through the analysis of doped ytterbium oxide nanoparticles.All these findings demonstrated that the ETSC provided a unique method for elemental and isotopic analysis of single nuclear particles.

关 键 词：多接收电感耦合等离子体质谱 单颗粒分析 单颗粒电感耦合等离子体质谱 稀土颗粒 模拟核颗粒 

分 类 号：O657.63[理学—分析化学] X830[理学—化学]