Institute of Inorganic and Analytical Chemistry, Justus Liebig University Giessen, Heinrich Buff Ring 17, 35392, Giessen, Germany.
Anal Bioanal Chem. 2021 Oct;413(24):5927-5948. doi: 10.1007/s00216-021-03425-1. Epub 2021 Jun 18.
Metabolomics and lipidomics are new drivers of the omics era as molecular signatures and selected analytes allow phenotypic characterization and serve as biomarkers, respectively. The growing capabilities of untargeted and targeted workflows, which primarily rely on mass spectrometric platforms, enable extensive charting or identification of bioactive metabolites and lipids. Structural annotation of these compounds is key in order to link specific molecular entities to defined biochemical functions or phenotypes. Tandem mass spectrometry (MS), first and foremost collision-induced dissociation (CID), is the method of choice to unveil structural details of metabolites and lipids. But CID fragment ions are often not sufficient to fully characterize analytes. Therefore, recent years have seen a surge in alternative tandem MS methodologies that aim to offer full structural characterization of metabolites and lipids. In this article, principles, capabilities, drawbacks, and first applications of these "advanced tandem mass spectrometry" strategies will be critically reviewed. This includes tandem MS methods that are based on electrons, photons, and ion/molecule, as well as ion/ion reactions, combining tandem MS with concepts from optical spectroscopy and making use of derivatization strategies. In the final sections of this review, the first applications of these methodologies in combination with liquid chromatography or mass spectrometry imaging are highlighted and future perspectives for research in metabolomics and lipidomics are discussed.
代谢组学和脂质组学是组学时代的新驱动力，因为分子特征和选定的分析物分别允许表型特征化，并作为生物标志物。非靶向和靶向工作流程的能力不断增强，这些工作流程主要依赖于质谱平台，能够广泛绘制或识别生物活性代谢物和脂质。为了将特定的分子实体与定义的生化功能或表型联系起来，对这些化合物进行结构注释是关键。串联质谱（MS），首先是碰撞诱导解离（CID），是揭示代谢物和脂质结构细节的首选方法。但是，CID 碎片离子通常不足以完全表征分析物。因此，近年来出现了许多替代的串联 MS 方法，旨在提供代谢物和脂质的完整结构表征。本文将批判性地回顾这些“高级串联质谱”策略的原理、能力、缺点和初步应用。这包括基于电子、光子和离子/分子的串联 MS 方法，以及离子/离子反应，将串联 MS 与光学光谱学的概念相结合，并利用衍生化策略。在本文的最后部分，强调了这些方法与液相色谱或质谱成像相结合的初步应用，并讨论了代谢组学和脂质组学研究的未来展望。
