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Development of proton-transfer reaction mass spectrometry techniques : detection of trace gases in biology and medicine

机译:质子转移反应质谱技术的发展:生物学和医学中痕量气体的检测

摘要

The measurement of small quantities of gases and volatiles in air is used nowadays in many different fields of science, such as chemistry, physics, biology, food science and medicine. The study of these minute quantities of gases requires highly sensitive detectors. Using such detectors to monitor the emission of molecules can provide useful insight into processes inside the emitter. However, the sources, amounts and types of volatile organic compounds can vary greatly, requiring different types of dedicated or highly versatile detectors. This thesis is about the development and application of trace gas detectors based on mass spectrometers. To be more specific, products of chemical reactions of trace gas molecules with H3O+ ions are studied. This experimental technique is called Proton-Transfer Reaction Mass Spectrometry (PTR-MS). The nature of the proton-transfer reaction enables the detection of extremely low levels (i.e. at (sub-) ppbv level; 1:1.000.000.000) of many different types of trace gases at a high time resolution. This thesis includes a description of the thermodynamics and chemistry behind the PTR-MS technique and contains a large variety of studies in different areas of application. These examples include the study of biological processes in plants and fruits and the quest for biomarkers of diseases in human breath. Besides the application of the PTR-MS technique, this thesis also contains a description of the development of a new type of PTR-MS detector, equipped with an ion trap mass spectrometer instead of the conventional quadrupole mass filter. This new system is shown to provide highly improved possibility of identification of detected volatile organic compounds.
机译:如今,在许多不同的科学领域,例如化学,物理,生物学,食品科学和医学中,都使用空气中少量气体和挥发物的测量方法。对这些微量气体的研究需要高度灵敏的检测器。使用此类检测器监视分子的发射可以提供对发射器内部过程的有用了解。但是,挥发性有机化合物的来源,数量和类型可能相差很大,需要使用不同类型的专用或高度通用的检测器。本文是关于基于质谱仪的痕量气体检测仪的开发与应用。更具体地说,研究了痕量气体分子与H3O +离子的化学反应产物。这种实验技术称为质子转移反应质谱(PTR-MS)。质子转移反应的性质使得能够以高的时间分辨率检测许多不同类型的痕量气体的极低水平(即(亚)ppbv水平; 1:1.000.000.000)。本论文包括对PTR-MS技术背后的热力学和化学的描述,并且在不同的应用领域进行了大量的研究。这些例子包括对植物和水果中生物过程的研究以及对人类呼吸疾病的生物标志物的追求。除了应用PTR-MS技术外,本文还描述了新型PTR-MS检测器的发展,该检测器配备了离子阱质谱仪代替了传统的四极杆质量过滤器。该新系统显示出可大大提高鉴定检测到的挥发性有机化合物的可能性。

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