Abstract

Background

High resolution mass spectrometry (HRMS) is being used increasingly in the context of suspect and non-targeted screening for the identification of bioorganic molecules. There is correspondingly increasing awareness that higher confidence identification will require a systematic, group effort to increase the fraction of compounds with tandem mass spectra available in central, publicly available resources. While typical suspect screening efforts will only result in tentative annotations with a moderate level of confidence, library spectral matches will yield higher confidence or even full confirmation of the identity if the reference standards are available.

Results

This article first explores representative percent coverage of measured tandem mass spectra in selected major environmental suspect databases of interest in the context of human biomonitoring, demonstrating the current extensive gap between the number of potential substances of interest (up to hundreds of thousands) and measured spectra (0.57–3.6% of the total chemicals have spectral information available). Furthermore, certain datasets are benchmarked, based on previous efforts, to show the extent to which acquired experimental data were comparable between laboratories, even with HRMS instruments based on different technologies (i.e., quadrupole–quadrupole-time of flight versus ion trap/quadrupole-Orbitrap). Instruments and settings that are less comparable are also revealed, primarily linear ion trap instruments, which show distinctly lower comparability.

Conclusions

Based on these efforts, harmonization guidelines for the acquisition and processing of tandem mass spectrometry data are proposed to enable European (and ideally worldwide) laboratories to contribute to common resources, without requiring extensive changes to their current in house methods.

中文翻译：

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关于串联质谱库的质量控制和质量保证的欧洲提案

摘要

背景

高分辨率质谱法（HRMS）越来越多地用于可疑和非靶向筛选的生物有机分子鉴定。相应地，人们越来越认识到，更高的置信度鉴定将需要系统的，集体的努力，以增加可从中央，公众获得的资源中获得的具有串联质谱的化合物的比例。尽管典型的可疑筛查工作只会产生具有中等置信度的暂定注释，但如果有参考标准，则谱库光谱匹配将产生更高的置信度，甚至可以完全确认身份。

结果

本文首先探讨了在人类生物监测背景下选定的主要环境可疑数据库中测量串联质谱的代表性百分比覆盖率，证明了潜在的潜在物质数量（多达数十万）和测量光谱之间的当前巨大差距（占总化学品的0.57–3.6％具有可用的光谱信息）。此外，根据以前的努力，对某些数据集进行了基准测试，以显示实验室之间获得的实验数据在何种程度上具有可比性，即使使用基于不同技术的HRMS仪器（例如，四极杆-四极杆飞行时间与离子阱/四极杆-飞行时间， Orbitrap）。还揭示了可比性较差的仪器和设置，主要是线性离子阱仪器，

结论

在这些努力的基础上，提出了用于采集和处理串联质谱数据的统一准则，以使欧洲（最好是全球范围内）的实验室能够为公共资源做出贡献，而无需对其现有内部方法进行大量更改。