通过热脱附二次电喷雾电离质谱法进行高通量挥发性脂肪酸皮肤代谢物分析。

High throughput volatile fatty acid skin metabolite profiling by thermal desorption secondary electrospray ionisation mass spectrometry.

作者信息

Martin Helen J, Reynolds James C, Riazanskaia Svetlana, Thomas C L Paul

机构信息

Centre for Analytical Science, Department of Chemistry, Loughborough University, Loughborough, Leicestershire LE11 3TU, UK.

出版信息

Analyst. 2014 Sep 7;139(17):4279-86. doi: 10.1039/c4an00134f.

Abstract

The non-invasive nature of volatile organic compound (VOC) sampling from skin makes this a priority in the development of new screening and diagnostic assays. Evaluation of recent literature highlights the tension between the analytical utility of ambient ionisation approaches for skin profiling and the practicality of undertaking larger campaigns (higher statistical power), or undertaking research in remote locations. This study describes how VOC may be sampled from skin and recovered from a polydimethylsilicone sampling coupon and analysed by thermal desorption (TD) interfaced to secondary electrospray ionisation (SESI) time-of-flight mass spectrometry (MS) for the high throughput screening of volatile fatty acids (VFAs) from human skin. Analysis times were reduced by 79% compared to gas chromatography-mass spectrometry methods (GC-MS) and limits of detection in the range 300 to 900 pg cm(-2) for VFA skin concentrations were obtained. Using body odour as a surrogate model for clinical testing 10 Filipino participants, 5 high and 5 low odour, were sampled in Manilla and the samples returned to the UK and screened by TD-SESI-MS and TD-GC-MS for malodour precursors with greater than >95% agreement between the two analytical techniques. Eight additional VFAs were also identified by both techniques with chains 4 to 15 carbons long being observed. TD-SESI-MS appears to have significant potential for the high throughput targeted screening of volatile biomarkers in human skin.

摘要

从皮肤采集挥发性有机化合物(VOC)具有非侵入性,这使其成为新型筛查和诊断检测方法开发的重点。对近期文献的评估凸显了用于皮肤分析的常压电离方法的分析实用性与开展更大规模研究(更高统计效力)或在偏远地区开展研究的实际可行性之间的矛盾。本研究描述了如何从皮肤采集VOC,并从聚二甲基硅氧烷采样片上回收,然后通过与二次电喷雾电离(SESI)飞行时间质谱(MS)联用的热脱附(TD)进行分析,以高通量筛查人皮肤中的挥发性脂肪酸(VFA)。与气相色谱 - 质谱法(GC - MS)相比,分析时间减少了79%,并获得了VFA皮肤浓度在300至900 pg cm(-2)范围内的检测限。以体臭作为临床测试的替代模型,对10名菲律宾参与者(5名高体味者和5名低体味者)在马尼拉进行采样,样本带回英国后,通过TD - SESI - MS和TD - GC - MS对恶臭前体进行筛查,两种分析技术之间的一致性大于95%。两种技术还鉴定出另外8种VFA,观察到其碳链长度为4至15个碳。TD - SESI - MS在高通量靶向筛查人皮肤中的挥发性生物标志物方面似乎具有巨大潜力。

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