Rapid in vivo fingerprinting of nonvolatile compounds in breath by extractive electrospray ionization quadrupole time-of-flight mass spectrometry
Rapid in vivo fingerprinting of nonvolatile compounds in breath by extractive electrospray ionization quadrupole time-of-flight mass spectrometry
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DOI：
10.1002/anie.200602942
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发表时间：
2007-01-01
影响因子：
16.6
通讯作者：
Zenobi, Renato
中科院分区：
文献类型：
--
作者：
Chen, Huanwen;Wortmann, Arno;Zenobi, Renato
呼出气体中微量成分的定量分析可以提供对体内生化过程的有用洞察[1-7]，从而揭示有关代谢动力学的信息，并在理论上为生物标志物研究[4，8]或临床诊断提供科学基础。然而，由于分析困难，在临床医学中很少将呼吸用于诊断目的。使用质子转移反应质谱仪(PTR-MS)、[10-12]选择离子流管(SIFT)[5-7]质谱仪等方法对快速呼气分析进行了许多尝试。和呼气冷凝液(EBC)分析，后者基于色谱分离。[11，15-18]然而，这些方法需要繁琐的样品采集[3，19-21]和样品前处理程序。[8，10，16，22，23]PTR-MS[10]和SIFT-MS[5，7]已用于直接呼气分析，但需要特殊设计的仪器，但这些仪器并不广泛使用。到目前为止，在呼气中只检测到低分子化合物(高达约100Da)，[5-7]几乎完全是挥发性物质。除了SIFT-MS，呼吸中的高水分也会影响测量。[2，3，8]实际上，呼吸是一种气溶胶，除了挥发性成分外，还含有大量溶解在微滴中的非挥发性化合物。[24，25]我们在此报告了一种萃取式电喷雾电离(EESI)[26]四极飞行时间质谱仪(QTOF-MS)方法，该方法无需修改商用ESI界面(如图1所示)即可建立人体呼气的活体指纹图谱。它提供了一种直接探测人体代谢动力学的方法，并为口腔异味的快速临床诊断提供了一种简单、实验方便的方法。
Quantitative analysis of trace constituents in exhaled gas can provide useful insights into biochemical processes [1–7] in the body, thus revealing information about metabolic dynamics and providing, theoretically, a scientific base for biomarker research [4, 8] or clinical diagnoses.[2, 8, 9] Breath, however, is rarely used practically for diagnostic purposes in clinical medicine because of analytical difficulties.[2, 8] Numerous attempts have been made for fast breath analysis by using methods that include proton transfer reaction mass spectrometry (PTR-MS),[10–12] selected ion flow tube (SIFT)[5–7] mass spectrometry, and exhaled breath condensate (EBC) analysis,[3, 13, 14] the latter being based on chromatographic separation.[11, 15–18] However, these methods require tedious sample collection [3, 19–21] and sample pretreatment procedures.[8, 10, 16, 22, 23] PTR-MS [10] and SIFT-MS [5, 7] have been used for direct breath analysis, but require specially designed instruments that are not widely available. To date, only lowmolecular-weight compounds (up to ca. 100 Da),[5–7] almost exclusively volatile species, have been detected in breath. With the exception of SIFT-MS, measurements are also compromised by the high water content in breath.[2, 3, 8] Actually, breath is a type of aerosol, and, in addition to volatile constituents, contains a vast variety of nonvolatile compounds dissolved in the microdroplets.[24, 25] We herein report an extractive electrospray ionization (EESI)[26] quadrupole time-of-flight mass spectrometry (QTOF-MS) method that has been established without modification of a commercial ESI interface (shown schematically in Figure 1) for the rapid in vivo fingerprinting of human breath. It presents a direct way to probe the dynamics of body metabolism and a simple, experimentally convenient method for the fast clinical diagnosis of oral malodors, based on