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首页> 外文期刊>Journal of mass spectrometry: JMS >Atmospheric pressure chemical ionization of explosives induced by soft X-radiation in ion mobility spectrometry: mass spectrometric investigation of the ionization reactions of drift gasses, dopants and alkyl nitrates
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Atmospheric pressure chemical ionization of explosives induced by soft X-radiation in ion mobility spectrometry: mass spectrometric investigation of the ionization reactions of drift gasses, dopants and alkyl nitrates

机译：离子迁移谱法中通过软X射线诱导的炸药的大气压化学电离：漂移气体，掺杂剂和烷基硝酸盐的电离反应的质谱研究

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摘要

A promising replacement for the radioactive sources commonly encountered in ion mobility spectrometers is a miniaturized, energy-efficient photoionization source that produce the reactant ions via soft X-radiation (2.8 keV). In order to successfully apply the photoionization source, it is imperative to know the spectrum of reactant ions and the subsequent ionization reactions leading to the detection of analytes. To that end, an ionization chamber based on the photoionization source that reproduces the ionization processes in the ion mobility spectrometer and facilitates efficient transfer of the product ions into a mass spectrometer was developed. Photoionization of pure gasses and gas mixtures containing air, N-2, CO2 and N2O and the dopant CH2Cl2 is discussed. The main product ions of photoionization are identified and compared with the spectrum of reactant ions formed by radioactive and corona discharge sources on the basis of literature data. The results suggest that photoionization by soft X-radiation in the negative mode is more selective than the other sources. In air, adduct ions of O-2 - with H2O and CO2 were exclusively detected. Traces of CO2 impact the formation of adduct ions of O-2 - and Cl -(upon addition of dopant) and are capable of suppressing them almost completely at high CO2 concentrations. Additionally, the ionization products of four alkyl nitrates (ethylene glycol dinitrate, nitroglycerin, erythritol tetranitrate and pentaerythritol tetranitrate) formed by atmospheric pressure chemical ionization induced by X-ray photoionization in different gasses (air, N-2 and N2O) and dopants (CH2Cl2, C2H5Br and CH3I) are investigated. The experimental studies are complemented by density functional theory calculations of the most important adduct ions of the alkyl nitrates (M) used for their spectrometric identification. In addition to the adduct ions [M + NO3](-) and [M + Cl](-), adduct ions such as [M + N2O2](-), [M + Br](-) and [M+ I](-) were detected, and their gas-phase structures and energetics are investigated by density functional theory calculations. Copyright (C) 2016 John Wiley & Sons, Ltd.
机译：离子迁移谱仪中常见的放射性源的有希望的替代方法是小型化，高能效的光电离源，它通过软X射线辐射（2.8 keV）产生反应离子。为了成功应用光电离源，必须知道反应物离子的光谱以及随后导致检测分析物的电离反应。为此，开发了一种基于光电离源的电离室，该室可重现离子迁移谱仪中的电离过程，并有助于将产物离子有效转移到质谱仪中。讨论了纯净气体以及包含空气，N-2，CO2和N2O以及掺杂剂CH2Cl2的气体混合物的光电离。在文献数据的基础上，确定了光电离的主要产物离子，并将其与由放射性和电晕放电源形成的反应物离子光谱进行了比较。结果表明，在负模下通过软X射线进行的光电离比其他离子源更具选择性。在空气中，仅检测到O-2-与H2O和CO2的加成离子。痕量的二氧化碳会影响O-2-和Cl-（在添加掺杂剂时）加成离子的形成，并能够在高CO2浓度下几乎完全抑制它们。此外，在不同的气体（空气，N-2和N2O）和掺杂剂（CH2Cl2）中，X射线光电离引起的大气压化学电离形成了四种烷基硝酸盐（乙二醇二硝酸盐，硝酸甘油，赤藓糖醇四硝酸盐和季戊四醇四硝酸盐）的电离产物。 ，C2H5Br和CH3I）。实验研究得到了密度泛函理论计算的补充，这些理论是用于烷基硝酸盐（M）光谱鉴定的最重要加合物离子。除了加成离子[M + NO3]（-）和[M + Cl]（-）外，诸如[M + N2O2]（-），[M + Br]（-）和[M + I]等加成离子检测到（-），并通过密度泛函理论计算研究它们的气相结构和高能学。版权所有（C）2016 John Wiley＆Sons，Ltd.

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