Investigating the Potential of Drift Tube Ion Mobility for the Analysis of Oxidized Lipids.
Katyeny Manuela da SilvaMichele WölkPalina NepachalovichElias IturrospeAdrian CovaciAlexander L N van NuijsMaria FedorovaPublished in: Analytical chemistry (2023)
Epilipids, a subset of the lipidome that comprises oxidized, nitrated, and halogenated lipid species, show important biochemical activity in the regulation of redox lipid metabolism by influencing cell fate decisions, including death, health, and aging. Due to the large chemical diversity, reversed-phase liquid chromatography-high-resolution mass spectrometry (RPLC-HRMS) methods have only a limited ability to separate numerous isobaric and isomeric epilipids. Ion mobility spectrometry (IMS) is a gas-phase separation technique that can be combined with LC-HRMS to improve the overall peak capacity of the analytical platform. Here, we illustrate the advantages and discuss the current limitations of implementing IMS in LC-HRMS workflows for the analysis of oxylipins and oxidized complex lipids. Using isomeric mixtures of oxylipins, we demonstrated that while deprotonated ions of eicosanoids were poorly resolved by IMS, sodium acetate and metal adducts (e.g., Li, Na, Ag, Ba, K) of structural isomers often showed ΔCCS% above 1.4% and base peak separation with high-resolution demultiplexing (HRDm). The knowledge of the IM migration order was also used as a proof of concept to help in the annotation of oxidized complex lipids using HRDm and all-ion fragmentation spectra. Additionally, we used a mixture of deuterium-labeled lipids for a routine system suitability test with the purpose of improving harmonization and interoperability of IMS data sets in (epi)lipidomics.
Keyphrases
- high resolution mass spectrometry
- liquid chromatography
- mass spectrometry
- tandem mass spectrometry
- ultra high performance liquid chromatography
- high resolution
- low density lipoprotein
- fatty acid
- simultaneous determination
- gas chromatography
- solid phase extraction
- cell fate
- healthcare
- electronic health record
- public health
- quantum dots
- mental health
- clinical practice
- quality improvement
- human health
- high throughput
- risk assessment
- rna seq
- computed tomography
- ionic liquid
- social media
- single cell
- deep learning
- climate change
- data analysis
- molecular dynamics