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首页> 外文学位 >Gas-phase studies of distonic meta-benzyne and carbon-nitrogen ortho-benzyne analogues in a Fourier-transform ion cyclotron resonance (FT-ICR) mass spectrometer and in a flowing-afterglow-triple quadrupole (FA-QqQ) apparatus.
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Gas-phase studies of distonic meta-benzyne and carbon-nitrogen ortho-benzyne analogues in a Fourier-transform ion cyclotron resonance (FT-ICR) mass spectrometer and in a flowing-afterglow-triple quadrupole (FA-QqQ) apparatus.

机译：在傅立叶变换离子回旋共振（FT-ICR）质谱仪和流动余辉三重四极杆（FA-QqQ）装置中，对中子元间联苯和碳氮原联苯类似物的气相研究。

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摘要

Fourier-transform ion cyclotron resonance (FT-ICR) mass spectrometry was employed for the majority of the work discussed in this thesis due to its powerful capabilities. Distonic benzyne ions' reactivities were examined in the gas phase utilizing the FT-ICR, thereby avoiding difficulties associated with the short-lived nature of these highly reactive species in the condensed phase. High-level molecular orbital calculations were employed to help rationalize experimental results.;It has been discovered in our laboratories that some benzyne precursor molecules yield a carbon-nitrogen (CN) ortho-benzyne instead of the desired benzyne. Therefore, a flowing-afterglow-triple quadrupole (FA-QqQ) apparatus was employed to determine the energy thresholds for formation of several CN ortho-benzynes. The results of this study help to rationalize the facile formation of the CN ortho-benzyne moiety. This understanding can be applied to prevent or exploit the formation of the CN ortho-benzyne moiety in the gas phase.;Lastly, an investigation into the gas-phase reactivity of metal ion nitrene adducts was conducted. The reactions of the Mg+ and Cu + nitrene adducts with varying substrates involve radical and nonradical pathways, respectively, yielding characteristic reaction products for each adduct. This preliminary result suggests that the reactivity of metal ion nitrene adducts is strongly influenced by the type of the metal ion.
机译：傅立叶变换离子回旋共振质谱（FT-ICR）由于其强大的功能而被用于本论文的大部分工作。使用FT-ICR在气相中检查了爆炸性的苯炔离子的反应性，从而避免了与这些高反应性物种在冷凝相中具有短暂寿命有关的困难。高水平的分子轨道计算被用来帮助合理化实验结果。；在我们的实验室中发现，某些苯炔前体分子会产生碳氮（CN）邻苯甲醛，而不是所需的苯炔。因此，采用流动余辉三重四极杆（FA-QqQ）装置来确定形成多个CN邻苯并苯的能量阈值。这项研究的结果有助于合理化CN邻苯并zy部分的简便形成。该理解可用于防止或利用气相中CN邻-苄基部分的形成。最后，对金属离子氮烯加合物的气相反应性进行了研究。 Mg +和Cu +氮杂加合物与不同底物的反应分别涉及自由基和非自由基途径，从而为每种加合物生成特征性的反应产物。该初步结果表明，金属离子腈加合物的反应性受金属离子类型的强烈影响。

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  • 作者

    Yurkovich, Michael James.;

  • 作者单位

    Purdue University.;

  • 授予单位 Purdue University.;
  • 学科 Chemistry Analytical.
  • 学位 Ph.D.
  • 年度 2008
  • 页码 138 p.
  • 总页数 138
  • 原文格式 PDF
  • 正文语种 eng
  • 中图分类
  • 关键词

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