On mass ambiguities in high-resolution shotgun lipidomics

Item Type:	Article
Title:	On mass ambiguities in high-resolution shotgun lipidomics
Creators Name:	Bielow, C. and Mastrobuoni, G. and Orioli, M. and Kempa, S.
Abstract:	Mass-spectrometry based lipidomics aims to identify as many lipid species as possible from complex biological samples. Due to the large combinatorial search-space unambiguous identification of lipid species is far from trivial. Mass ambiguities are common in direct-injection shotgun experiments, where an orthogonal separation (e.g. liquid chromatography) is missing. Using the rich information of available lipid databases, we generated a comprehensive rule set describing mass ambiguities, while taking into consideration the resolving power (and its decay) of different mass analyzers. Importantly, common adduct species and isotopic peaks are accounted for and are shown to play a major role, both for perfect mass overlaps due to identical sum formulae as well as resolvable mass overlaps. We identified known and hitherto unknown mass ambiguities in high- and ultra-high resolution data, while also ranking lipid classes by their propensity to cause ambiguities. Based on this new set of ambiguity rules, guidelines and recommendations for experimentalists and software developers of what constitutes a solid lipid identification in both MS and MS/MS were suggested. For researchers new to the field, our results are a compact source of ambiguities which should be accounted for. These new findings also have implications for the selection of internal standards, peaks used for internal mass calibration, optimal choice of instrument resolution and sample preparation for example in regard to adduct ion formation.
Keywords:	Adipose Tissue, Factual Databases, High Pressure Liquid Chromatography, Lipids, Liver, Muscles, Sodium, Tandem Mass Spectrometry, Animals, Rats
Source:	Analytical Chemistry
ISSN:	0003-2700
Publisher:	American Chemical Society
Volume:	89
Number:	5
Page Range:	2986-2994
Date:	7 March 2017
Official Publication:	https://doi.org/10.1021/acs.analchem.6b04456
PubMed:	View item in PubMed

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