常压电离质谱在公共安全化学毒物检测的应用

常压电离质谱技术(Ambient ionization mass spectrometry,AIMS)以其敞开式环境、简便操作、原位、实时、高通量等优势,成为公共安全化学毒物检测领域的研究热点。该文基于文献计量分析,简要概述了AIMS的分类、发展趋势及其在公共安全化学毒物检测领域的发展现状,重点从检测灵敏度、样品前处理兼容性以及现场检测的小型化质谱适配性等方面,归类总结了AIMS在毒品、爆炸物、化学战剂和生物毒素等分析检测方面的应用特点,最后对其技术特点及未来发展待解决问题等进行了评述,为相关领域研究人员提供有益参考。     

原位电离-离子迁移谱法现场快速筛查玩具中5种酚类化合物北大核心CSCD

采用原位电离-离子迁移谱法现场快速筛查玩具中5种酚类化合物。玩具样品无需前处理,采用萃取纳升喷雾或纸喷雾原位电离方式,在11 ms内完成离子迁移谱法的检测,5种酚类化合物的检出限(3S/N)在0.5~1.5mg·kg^(-1)之间。筛查出的疑似阳性样品,进一步采用高效液相色谱-串联质谱法进行确证。     

原位电离-离子迁移谱法现场快速筛查玩具中5种酚类化合物

采用原位电离-离子迁移谱法现场快速筛查玩具中5种酚类化合物。玩具样品无需前处理,采用萃取纳升喷雾或纸喷雾原位电离方式,在11 ms内完成离子迁移谱法的检测,5种酚类化合物的检出限(3S/N)在0.5~1.5mg·kg~(-1)之间。筛查出的疑似阳性样品,进一步采用高效液相色谱-串联质谱法进行确证。     

实时直接分析质谱在农药检测中的应用

实时直接分析(Direct analysis in real time,DART)作为一种原位电离技术发展迅猛,其与质谱联用已成为热门的分析技术并广泛应用于法庭科学领域,如食品安全、爆炸物检测、毒物毒品分析和药物分析等方面。目前农药的常规检测方法已非常成熟,但引入原位电离-质谱联用技术可以拓宽检测范围,缩短检测时限。该文从实时直接分析质谱(DART-MS)技术的工作原理、检测条件优化及其在农药检测方面的应用进行综述,并对DART-MS的应用前景进行了展望。     

离子迁移谱仪6秒钟让爆炸物显露原形

不久前,中科院大连化学物理研究所成功研制可检测爆炸物和毒品的非放射性光电离源离子迁移谱仪,成功通过公安部检测。该仪器可满足大部分爆炸物和毒品检测种类的检测,6 s 即可检测出危险物,为公共安全现场快速分析提供有力保障。     

基于敞开式直接电离质谱技术的尿液中毒品检测北大核心CSCD

尿液作为一种易于获取的体内毒品检材,在吸毒人员快速筛查中被广泛应用。针对传统快速筛查技术存在假阳性率高、定量能力不足以及实验室质谱技术在快速检测中存在前处理复杂、检测耗时长、使用环境苛刻等问题,该文提出了一种基于敞开式直接电离质谱技术的生物样本快速检测方法。该研究采用探针式电喷雾离子源与便携式质谱仪联用快速检测平台,优化了喷雾电压和质谱入口毛细管温度,开发了高效快速的前处理技术。基于该平台和前处理技术,5种常规毒品(甲基苯丙胺、氯胺酮、可卡因、O^(6)-单乙酰吗啡和3,4-亚甲双氧甲基苯丙胺)的尿液加标溶液的检出限为0.5~30 ng/mL,且其中4种毒品定量检测的线性相关系数大于0.99。除此之外,5种常规毒品在3个不同水平下的加标回收率为56.1%~103.7%,多次检测结果的相对标准偏差为9.0%~27.8%,说明联用检测平台与前处理方法结合可以达到良好的准确度。为了进一步检验该联用仪器的实战能力,测试了某社区戒毒康复中心40份阳性和110份阴性实际尿液样本,总体检测的准确率接近99%,且通过一次进样在20 s内可同时检测多种毒品。该研究成果有利于推动快速检测技术的发展,促进敞开式直接电离质谱仪技术的推广应用,提升一线执法服务水平。     

基于机器学习的直接电离质谱爆炸物检测方法

直接电离质谱系统在现场快速检测中的应用日益广泛,主要用于爆炸物、毒品、食品添加剂等的检测。然而,直接电离质谱系统中质谱信号波动大且同一浓度样品峰强呈现对数正态分布,严重影响了检出限附近低浓度样品的检测准确性。该研究将乙酰水杨酸(115个样品)作为爆炸物模拟物,利用介质阻挡放电离子源与质谱系统,研究了基于机器学习的直接电离质谱数据预处理和分类算法,以提高低浓度样品的检测准确率。对两种浓度为1 ng/mL的常见爆炸物样本(三硝基甲苯和硝酸铵分别为110、90个)及空白对照样本(366个)开展了应用实验。结果表明,与传统提取离子流方法和高斯混合模型方法相比,采用随机森林算法可将F_score从0.74、0.89提升至0.96,显著提高了检测准确率,且单个样本数据分析时间远少于0.1 s,满足实时检测需求。     

纸喷雾敞开式质谱法的发展和应用

纸喷雾质谱法是一种新型的敞开式质谱技术,其以低价易处理的纸为载体,将样品加在三角形的纸上,通过施加高电压,目标分子在电场的驱动下到达纸尖,瞬间气化形成电喷雾,样品离子化后进入质谱进行分析。它具有敞开式质谱法和电喷雾电离技术的特点,可以在开放式大气压环境下对样品或样品表面的物质进行分析,分析成本低、高通量、简便、实时、快速,可简化工作流程,提高质谱仪器的易用性。本文从纸喷雾质谱法的原理出发,介绍了影响其电离效率的主要因素(如载体基质,溶剂系统,洗脱方式等),并对近几年该技术的改进和发展,及其在生物样品检测、植物化学分析、品种鉴别、食品安全和环境分析等领域的应用进行了综述,全面介绍了该项技术的特点和优势。多项研究证明纸喷雾质谱法是一个应用面广泛,具有很大发展前景的分析技术,对其开展研究工作十分有意义。最后讨论了纸喷雾质谱法存在的不足,并提出了相关改进的设想。     

常压直接离子化-离子迁移谱法快速筛查玩具中4种初级芳香胺

采用常压直接离子化结合离子迁移谱技术,研究并建立了蜡笔、纹身贴纸、液体玩具、手指画颜料、橡皮泥等多种玩具样品中2-萘胺、4-氯-2-甲基苯胺、4-氨基联苯和联苯胺4种初级芳香胺的现场快速筛查方法。样品无需经过繁琐的前处理过程,不同玩具样品采用纸喷雾、纳升萃取喷雾等常压直接离子化方法,将取样、萃取、电离等步骤集成为一步实现,并在12ms内完成离子迁移谱的仪器分析检测,4种初级芳香胺的方法检出限在0.5~2mg/kg之间。对于经离子迁移谱快速筛检出的疑似阳性样品,同时还建立了高效液相色谱-串联质谱确证方法。本方法快速便捷,适用于玩具质量安全现场快速筛查检测。     

常压电喷雾离子化的机理及应用

作为最有前景的分析仪器之一,质谱技术已在药物、食品、环境、人类健康、国家安全及相关领域展现出广阔的应用前景。不同种类的分析物具有多种特征,这为直接离子化及质谱分析增加了难度。常压敞开式离子源是近年来新兴的一种离子源,这类离子源具有无需复杂的样品前处理、操作方便、快速、非破坏性、灵敏度及特异性好、能实现实时原位、高通量分析等特点。本文综述了基于电喷雾离子化(ESI)原理的各种离子源的电离机理、特征及应用,展望了常压敞开式离子源的发展趋势。     

Research Advances in Ambient Ionization and Miniature Mass Spectrometry

The development and applications of ambient ionization and miniature mass spectrometry are current research focus in chemical measurement. The analytical technology based on the combination of ambient ionization and miniature mass spectrometry can bypass chromatographic separation and eliminate or simplify sample pretreatment process. The protocol can reverse the labor-intensive and time-consuming drawbacks of traditional analytical methodologies, and realize rapid, on-site analysis with high sensitivity and high throughput. In this paper, the research progress and applications of ambient ionization and miniature mass spectrometry in the fields of food safety, consumer product safety, public security, life sciences and environmental monitoring, are reviewed, and future trends and prospects are discussed, which may provide technical guidance for the researchers engaged in relevant fields.     

敞开式离子化质谱在贸易产品化学风险物质筛查中的应用及前景

敞开式离子化质谱是一种新兴的质谱快检技术,具有分析速度快、操作流程简单、特异性强等特点。该技术无需对样品做复杂预处理,尤其在与便携式质谱仪联用时,可用于大量样品的现场、快速、准确筛查,在贸易产品化学风险物质的筛查中展现出广泛的应用前景。该文主要综述敞开式离子化质谱近年来在贸易产品化学风险物质筛查方面的研究进展,并对其未来的发展前景进行了展望。     

Portable electrospray ionization mass spectrometry (ESI-MS) for analysis of contaminants in the field

Hitherto analysis of chemicals in the field using mass spectrometry (MS) has been limited to analysis of non-polar and thermally stabile organic compounds using either a direct gas leak or a membrane inlet as MS interface. Recently, Professor R. Graham Cooks’ group demonstrated that miniature mass spectrometers operating at elevated pressures (>0.13?Pa (1?·?10^?3??Torr)) can be combined with electrospray ionization (ESI) for analysis of polar as well as thermally labile organic compounds. We present a simple miniaturized ESI unit for analysis of small liquid samples using miniature mass spectrometry. The ESI unit operates without pumps and supplementary sheath gases, which makes it very simple to handle in the field. 20–30?µL of sample solution is simply dropped into a small cavity in the ESI unit, where after the spray is initiated by applying high voltage to it. The miniaturized ESI unit was tested in combination with a miniature mass spectrometer (the Mini 10 developed by Professor R. Graham Cooks, Purdue University, IN) and we found that common herbicides (Atrazine, Prometryne, Terbutryne and Triadimefone) could be detected with detection limits around 1?mg?L^?1 and with a quantitative reproducibility of +/?30%. These characteristics, although high for environmental samples, are comparable to detection limits obtained with other ESI units used with miniature mass spectrometers and represent an early step forward towards a future field instrument. A major advantage of the capillary spray cell is its direct compatibility with micro extraction techniques for sample pre-concentration.     

Ambient ionization mass spectrometry: a tutorial

Ambient ionization is a set of mass spectrometric ionization techniques performed under ambient conditions that allows the direct analysis of sample surfaces with little or no sample pretreatment. Using combinations of different types of sample introduction systems and ionization methods, several novel techniques have been developed over the last few years with many applications (e.g., food safety screening; detection of pharmaceuticals and drug abuse; monitoring of environmental pollutants; detection of explosives for antiterrorism and forensics; characterization of biological compounds for proteomics and metabolomics; molecular imaging analysis; and monitoring chemical and biochemical reactions). Electrospray ionization and atmospheric pressure chemical ionization are the two main ionization principles most commonly used in ambient ionization mass spectrometry. This tutorial paper provides a review of the publications related to ambient ionization techniques. We describe and compare the underlying principles of operation, ionization processes, detecting mass ranges, sensitivity, and representative applications of these techniques.     

Forensic applications of ambient ionization mass spectrometry

This review highlights and critically assesses forensic applications in the developing field of ambient ionization mass spectrometry. Ambient ionization methods permit the ionization of samples outside the mass spectrometer in the ordinary atmosphere, with minimal sample preparation. Several ambient ionization methods have been created since 2004 and they utilize different mechanisms to create ions for mass-spectrometric analysis. Forensic applications of these techniques—to the analysis of toxic industrial compounds, chemical warfare agents, illicit drugs and formulations, explosives, foodstuff, inks, fingerprints, and skin—are reviewed. The minimal sample pretreatment needed is illustrated with examples of analysis from complex matrices (e.g., food) on various substrates (e.g., paper). The low limits of detection achieved by most of the ambient ionization methods for compounds of forensic interest readily offer qualitative confirmation of chemical identity; in some cases quantitative data are also available. The forensic applications of ambient ionization methods are a growing research field and there are still many types of applications which remain to be explored, particularly those involving on-site analysis. Aspects of ambient ionization currently undergoing rapid development include molecular imaging and increased detection specificity through simultaneous chemical reaction and ionization by addition of appropriate chemical reagents.     

Recent developments of miniature ion trap mass spectrometers

The recent development of miniature ion trap mass spectrometer systems in the last ten years is reviewed in this paper. These instruments adopt different atmospheric pressure interfaces (APIs), which are membrane inlets (MIs), discontinuous atmospheric pressure interface (DAPI) and continuous atmospheric pressure interface (CAPI).     

In Situ Explosive Detection Using a Miniature Plasma Ion Source and a Portable Mass Spectrometer

A small low-temperature plasma (LTP) ionization probe was coupled to a portable mass spectrometer for the rapid detection of trace explosives on surfaces. Using only a small diaphragm pump to supply ambient air to the LTP source, 100 ng each of pentaerythritol tetranitrate (PETN), 1,3,5-trinitroperhydro-1,3,5-triazine (RDX), and 2,4,6-trinitrophenylmethylnitramine (Tetryl) were detectable on glass in under 1 minute. The main ion signal from these molecules (M) is the [M + NO₃]^? species. While much optimization remains, it is believed that this miniature LTP source will remove the need for external gas cylinders and additional heating for in situ explosives detection using portable mass spectrometers.     

介质阻挡放电离子源质谱分析

敞开式离子化质谱可对表面样品进行直接快速分析而受到关注,成为质谱分析的热点研究方向.介质阻挡放电离子源是一种基于等离子体放电机理的敞开式离子源,近年来得到了较快的发展.本文着重介绍该离子源的基本原理、性能特征以及应用进展,并对其发展趋势进行了展望.     

Non-proximate detection of explosives and chemical warfare agent simulants by desorption electrospray ionization mass spectrometry

Desorption electrospray ionization (DESI) mass spectrometry is used for the selective and sensitive detection of trace amounts of explosives and chemical warfare agent simulants from ambient surfaces at distances of up to 3 meters from the mass spectrometer.