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首页> 外文学位 >Characteristic ion /molecule reactions at low and at atmospheric pressure for selective detection of dangerous substances.
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Characteristic ion /molecule reactions at low and at atmospheric pressure for selective detection of dangerous substances.

机译：在低压和大气压下进行离子/分子反应的特征，用于选择性检测危险物质。

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摘要

Characteristic ion/molecule reactions are selective to substrates with a specific functionality and therefore are useful in enhancing the selectivity in the detection of trace organic compounds when coupled with mass spectrometry. Nitroaromatic compounds can be reduced to arylnitrenium ions by vinyl halide radical cations and can form σ-bonded Meisenheimer complexes with carbon/oxygen-centered anions in the gas phase due to their strong electron deficiency. Also, phosphonium ions were found to undergo selective ketalization with 1,4-dioxane. It has been demonstrated that explosives and chemical warfare agent simulants in mixtures can be selectively detected using these new characteristic ion/molecule reactions. Another characteristic ion/molecule reaction uncovered is the cycloaddition/cyclization of the TNT and RDX fragment ions with ethyl vinyl ether.;A thermal desorption-APCI method was also developed for the detection of explosives on solid surfaces, in which explosives were desorbed from the surface by rapid heating and then underwent ionization or ion/molecule reactions. In addition, a new atmospheric pressure thermal desorption ionization (APTDI) method was established for producing ions from organic ionic compounds by heating at atmospheric pressure. The effect of matrix and solvent on the ionization was examined.;While the ion/molecule reactions mentioned above were performed at low pressure inside the mass spectrometer, several ion/molecule reactions, such as Meisenheimer complexation, ketalization, conversion of pyrylium into pyridinium ion, Eberlin and deprotonation reactions, were also investigated in the gas phase at atmospheric pressure by employing ESI, APCI and APTDI with designed reactors.;Finally, stereoselective proton transfer reactions were successfully used for chiral recognition using tandem mass spectrometry. The hydrogen/chlorine exchange reaction between carbanion CH2NO2- and CCl4 is also studied.
机译：离子/分子反应对具有特定功能的底物具有选择性，因此在与质谱联用时可用于提高痕量有机化合物检测的选择性。硝基芳香族化合物可以通过乙烯基卤化物自由基阳离子还原为芳基氮离子，并且由于其强电子缺乏性，可以在气相中与以碳/氧为中心的阴离子形成σ键结合的Meisenheimer配合物。另外，发现phospho离子用1，4-二恶烷选择性缩酮化。已经证明，使用这些新的特征离子/分子反应可以选择性地检测混合物中的炸药和化学战剂模拟物。还发现了另一个特征性的离子/分子反应是TNT和RDX碎片离子与乙基乙烯基醚的环加成/环化。;还开发了一种热脱附-APCI方法来检测固体表面上的炸药，其中炸药从通过快速加热表面，然后进行电离或离子/分子反应。此外，建立了一种新的常压热脱附电离（APTDI）方法，用于通过在大气压下加热由有机离子化合物产生离子。检验了基质和溶剂对电离的影响。;虽然上述离子/分子反应是在质谱仪内部低压下进行的，但一些离子/分子反应如迈森海默络合，缩酮化，吡啶鎓转化为吡啶鎓离子等还通过在ESI，APCI和APTDI设计的反应器中在大气压下在气相中研究了Eberlin和去质子化反应;最后，通过串联质谱法成功地将立体选择性质子转移反应用于手性识别。还研究了碳负离子CH2NO2-和CCl4之间的氢/氯交换反应。

著录项

  • 作者

    Chen, Hao.;

  • 作者单位

    Purdue University.;

  • 授予单位 Purdue University.;
  • 学科 Chemistry Analytical.
  • 学位 Ph.D.
  • 年度 2005
  • 页码 234 p.
  • 总页数 234
  • 原文格式 PDF
  • 正文语种 eng
  • 中图分类
  • 关键词

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