In-Silico-Generated Library for Sensitive Detection of 2-Dimethylaminoethylamine Derivatized FAHFA Lipids Using High-Resolution Tandem Mass Spectrometry.
Jun DingTobias KindQuan-Fei ZhuYu WangJing-Wen YanOliver FiehnBi-Feng YuanPublished in: Analytical chemistry (2020)
Fatty acid esters of hydroxy fatty acids (FAHFAs) are a family of recently discovered lipids with important physiological functions in mammals and plants. However, low detection sensitivity in negative ionization mode mass spectrometry makes low-abundance FAHFA challenging to analyze. A 2-dimethylaminoethylamine (DMED) based chemical derivatization strategy was recently reported to improve the MS sensitivity of FAHFAs by labeling FAHFAs with a positively ionizable tertiary amine group. To facilitate reliable, high-throughput, and automatic annotation of these compounds, a DMED-FAHFA in silico library containing 4290 high-resolution tandem mass spectra covering 264 different FAHFA classes was developed. The construction of the library was based on the heuristic information from MS/MS fragmentation patterns of DMED-FAHFA authentic standards, and then, the patterns were applied to computer-generated DMED-FAHFAs. The developed DMED-FAHFA in silico library was demonstrated to be compatible with library search software NIST MS Search and the LC-MS/MS data processing tool MS-DIAL to guarantee high-throughput and automatic annotations. Applying the in silico library in Arabidopsis thaliana samples for profiling FAHFAs by high-resolution LC-MS/MS enabled the annotation of 19 DMED-FAHFAs from 16 families, including 3 novel compounds. Using the in silico library largely decreased the false-positive annotation rate in comparison to low-resolution LC-MS/MS. The developed library, MS/MS spectra, and development templates are freely available for commercial and noncommercial use at https://zenodo.org/record/3606905.
Keyphrases
- mass spectrometry
- ms ms
- high resolution
- tandem mass spectrometry
- liquid chromatography
- gas chromatography
- fatty acid
- high performance liquid chromatography
- ultra high performance liquid chromatography
- high throughput
- molecular docking
- sensitive detection
- simultaneous determination
- arabidopsis thaliana
- liquid chromatography tandem mass spectrometry
- single cell
- multiple sclerosis
- high resolution mass spectrometry
- rna seq
- deep learning
- capillary electrophoresis
- social media
- solid phase extraction
- loop mediated isothermal amplification
- density functional theory
- health information
- neural network
- clinical evaluation
- big data