Deep-lipidotyping by mass spectrometry: recent technical advances and applications

Zhang, Wenpeng; Jian, Ruijun; Zhao, Jing; Liu, Yikun; Xia, Yu

doi:10.1016/j.jlr.2022.100219

Cited by 36 publications

(38 citation statements)

References 124 publications

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“…These methods have been summarized in recent reviews on lipid analysis. 47,48 The formation of metal ion-adducted lipids has also been used to generate characteristic fragment ions for isomer identification. [49][50][51][52] Silver salts can bind lipids at CvC bonds which helps with CvC bond-positional determination.…”

Section: Introductionmentioning

confidence: 99%

Characterization of glycerophospholipids at multiple isomer levels via Mn(ii)-catalyzed epoxidation

Chen

Tang

Freitas

et al. 2022

Analyst

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Section: Introductionmentioning

confidence: 99%

Characterization of glycerophospholipids at multiple isomer levels via Mn(ii)-catalyzed epoxidation

Chen

Tang

Freitas

et al. 2022

Analyst

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“…Figure 4B demonstrates how a spectrum graph is constructed for a polyunsaturated chain. Four principle vertices, V (6, 1) , V (9, 2) , V (12,3) , V (15,4) , are identified from PB-MS 2 CID data of PE 37:4 (Figure 2B). Four paths are constructed with an increasing degree of unsaturation of a fatty acyl chain (Ω from 1 to 4): Path 1: V S -V (6, 1) -V E ; Path 2: V S -V (6, 1) -V (9, 2) -V E ; Path 3: V S -V (6, 1) -V (9, 2) -V (12, 3) -V E ; Path 4: V S -V (6, 1) -V (9, 2) -V (12, 3) -V (15,4) -V E .…”

Section: ■ Results and Discussionmentioning

confidence: 99%

“…Increasing evidence reveals that the compositions of lipid CC location isomers vary in cancer cells or tissues due to dysregulation of key desaturation enzymes in lipid metabolism. , Lipidome-wide identification and quantitation of lipids at CC location level thus can facilitate disease phenotyping and lipid marker discovery. , High-resolution mass spectrometry (HRMS) and tandem mass spectrometry (MS/MS) are routinely used to profile lipids at the sum composition and chain composition levels; , however, they fail to locate CCs in unsaturated lipids via low-energy collision-induced dissociation (CID). In the past decade, new gas-phase dissociation methods have been explored and applied in locating CCs in lipids, such as ozone-induced dissociation (OzID), ,, electron impact excitation of ions from organics (EIEIO), , ultraviolent photon dissociation (UVPD), , and so on . Alternatively, CC specific chemical derivatizations which promote cleavage at the modified site via CID are also found effective to locate CC without requiring specialized mass spectrometers.…”

Section: Introductionmentioning

confidence: 99%

LipidOA: A Machine-Learning and Prior-Knowledge-Based Tool for Structural Annotation of Glycerophospholipids

et al. 2022

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The Paterno−Buchi (PB) reaction is a carbon− carbon double bond (C�C)-specific derivatization reaction that can be used to pinpoint the location(s) of C�C(s) in unsaturated lipids and quantitate the location of isomers when coupled with tandem mass spectrometry (MS/MS). As the data of PB-MS/MS are increasingly generated, the establishment of a corresponding data analysis tool is highly needed. Herein, LipidOA, a machine-learning and prior-knowledge-based data analysis tool, is developed to analyze PB-MS/MS data generated by liquid chromatography−mass spectrometry workflows. LipidOA consists of four key functional modules to realize an annotation of glycerophospholipid (GPL) structures at the fatty acyl-specific C�C location level. These include (1) data preprocessing, (2) picking C�C diagnostic ions, (3) de novo annotation, and (4) result ranking. Importantly, in the result-ranking module, the reliability of structural annotation is sorted via the use of a machine learning classifier and comparison to the total fatty acid database generated from the same sample. LipidOA is trained and validated by four PB-MS/MS data sets acquired using different PB reagents on mass spectrometers of different resolutions and of different biological samples. Overall, LipidOA provides high precision (higher than 0.9) and a wide coverage for structural annotations of GPLs. These results demonstrate that LipidOA can be used as a robust and flexible tool for annotating PB-MS/MS data collected under different experimental conditions using different lipidomic workflows.

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“…Although OzID has been used for the dissociation of CC of several classes of lipids in MS analysis, it was usually performed in positive-ion mode with a focus on lipid subclasses readily ionized in this modality, including PCs, SMs, phosphatidylethanolamines (PEs), triacylglycerols (TGs), and FAMEs . To date, there have been fewer reports of OzID analysis in negative-ion mode with some lipid subclasses examined in this modality, , such as fatty acid esters of hydroxy fatty acids (FAHFAs), exhibiting reduced reactivity . Encouraged by the efficiency gains of the miniature OzID MS system, we tried to identify the CC locations of unsaturated FAs by OzID in negative-ion mode.…”

Section: Resultsmentioning

confidence: 99%

Development of a Miniature Mass Spectrometry System for Point-of-Care Analysis of Lipid Isomers Based on Ozone-Induced Dissociation

Jiao

Cao

et al. 2022

Anal. Chem.

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Disorder of lipid homeostasis is closely associated with a variety of diseases. Although mass spectrometry (MS) approaches have been well developed for the characterization of lipids, it still lacks an integrated and compact MS system that is capable of rapid and detailed lipid structural characterization and can be conveniently transferred into different laboratories. In this work, we describe a novel miniature MS system with the capability of both ozone-induced dissociation (OzID) and collision-induced dissociation (CID) for the assignment of sites of unsaturation and sn-positions in glycerolipids. A miniature ozone generator was developed, which can be operated at a relatively high pressure. By maintaining high-concentration ozone inside the linear ion trap, OzID efficiency was significantly improved for the identification of CC locations in unsaturated lipids, with reaction times as short as 10 ms. Finally, the miniature OzID MS system was applied to the analysis of CC locations and sn-positions of lipids from biological samples. Direct sampling and fast detection of changes in phospholipid isomers were demonstrated for the rapid discrimination of breast cancer tissue samples, showing the potential of the miniature OzID MS system for point-of-care analysis of lipid isomer biomarkers in complex samples.

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Deep-lipidotyping by mass spectrometry: recent technical advances and applications

Cited by 36 publications

References 124 publications

Characterization of glycerophospholipids at multiple isomer levels via Mn(ii)-catalyzed epoxidation

Characterization of glycerophospholipids at multiple isomer levels via Mn(ii)-catalyzed epoxidation

LipidOA: A Machine-Learning and Prior-Knowledge-Based Tool for Structural Annotation of Glycerophospholipids

Development of a Miniature Mass Spectrometry System for Point-of-Care Analysis of Lipid Isomers Based on Ozone-Induced Dissociation

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