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Development and characterization of an inductively coupled plasma/electrospray ionization dual-source time-of-flight mass spectrometer.

机译:电感耦合等离子体/电喷雾电离双源飞行时间质谱仪的开发和表征。

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摘要

In recent years the importance of chemical speciation, i.e. the quantitative determination of an element amongst its various oxidation states and molecular or complex forms, has been recognized as more relevant than total elemental concentration. Although the total elemental concentration is often easier to evaluate, the bioavailability and toxicological information it yields is inherently limited. It has been demonstrated that identification based on chromatographic separation alone cannot provide sufficient qualitative information for native biological samples, due to the unknown nature of the sample. For this reason, researchers have begun employing two separate instruments to obtain the elemental and molecular information from such samples. However, employing separate instruments for the analysis of a given sample has several disadvantages. In the presented work, a single time-of-flight mass spectrometer (TOFMS) will be described that utilizes two ionization sources to obtain comprehensive atomic and molecular information simultaneously.;A dual-source TOFMS has been designed and constructed in our laboratory. The current arrangement for the instrument utilizes an inductively coupled plasma to obtain elemental, isotopic, and quantitative information. Meanwhile, an electrospray source is operated in parallel to provide molecular and structural information. Due to the wide mass range and high spectral-generation rate of TOFMS, ions from both sources can simultaneously be sampled by a single mass analyzer to provide excellent temporal resolution of transient signals, while simultaneously simplifying peak assignment from a chromatographic separation. Furthermore, since only a single chromatographic separation is necessary for the atomic and molecular channels, sample requirements, preparation time, and analysis time can be significantly reduced.
机译:近年来,已经认识到化学形态形成的重要性,即在各种氧化态和分子或复杂形式中定量确定一种元素比总元素浓度更重要。尽管总元素浓度通常更容易评估,但其产生的生物利用度和毒理学信息固有地受到限制。已经证明,由于样品的未知性质,仅基于色谱分离的鉴定不能为天然生物样品提供足够的定性信息。因此,研究人员已开始使用两种单独的仪器从此类样品中获取元素和分子信息。但是,采用单独的仪器分析给定的样品有几个缺点。在本文的工作中,将描述一个单飞行时间质谱仪(TOFMS),该质谱仪利用两个电离源同时获得全面的原子和分子信息。;双源TOFMS已在我们的实验室中设计和构建。该仪器的当前布置利用感应耦合等离子体来获得元素,同位素和定量信息。同时,电喷雾源并联运行以提供分子和结构信息。由于TOFMS的质量范围广且光谱产生速率高,因此可以通过单个质量分析仪同时采样来自两个离子源的离子,以提供出色的瞬态信号时间分辨率,同时简化了色谱分离过程中的峰分配。此外,由于原子和分子通道仅需进行一次色谱分离,因此可以显着减少样品需求,制备时间和分析时间。

著录项

  • 作者

    Rogers, Duane A.;

  • 作者单位

    Indiana University.;

  • 授予单位 Indiana University.;
  • 学科 Chemistry Analytical.
  • 学位 Ph.D.
  • 年度 2009
  • 页码 321 p.
  • 总页数 321
  • 原文格式 PDF
  • 正文语种 eng
  • 中图分类
  • 关键词

  • 入库时间 2022-08-17 11:37:46

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