Hydrogen-Deuterium Scrambling Based on Chemical Isotope Labeling Coupled with LC-MS: Application to Amine Metabolite Identification in Untargeted Metabolomics.
Shu-Jian ZhengJie ZhengCai-Feng XiongHua-Ming XiaoShi-Jie LiuBi-Feng YuanPublished in: Analytical chemistry (2020)
Identification of metabolites at the trace level in complex samples is still one of the major challenges in untargeted metabolomics. One formula in the metabolomic database is always corresponding to more than one candidate, which increases the difficulty and cost in the subsequent process of standard compound matching. In this study, we developed an effective method for amine metabolite identification by hydrogen-deuterium scrambling (HDS) based on chemical isotope labeling coupled with liquid chromatography-mass spectrometry (HDS-CIL-LC-MS). After d4-4-(N,N-dimethylamino)phenyl isothiocyanate (d4-DMAP) labeling, the labeled amine metabolites can produce HDS under collision-induced dissociation (CID). The HDS can effectively reflect the number of labile hydrogen atoms in amine metabolites and thus distinguish amine isomers with different functional groups. The developed HDS-CIL-LC-MS method was applied to the determination of amine metabolites in mice feces, in which the amine candidates obtained by the database based on chemical formula searching were reduced by 64% on average, which greatly reduces the cost of standard compound matching. Taken together, the developed HDS-CIL-LC-MS analysis was demonstrated to be a promising method for untargeted metabolomics and a novel strategy for deciphering tandem mass spectrometry (MS2) spectra.
Keyphrases
- mass spectrometry
- liquid chromatography
- tandem mass spectrometry
- gas chromatography
- high resolution mass spectrometry
- high performance liquid chromatography
- ultra high performance liquid chromatography
- solid phase extraction
- ms ms
- simultaneous determination
- capillary electrophoresis
- high resolution
- gas chromatography mass spectrometry
- oxidative stress
- computed tomography
- type diabetes
- molecularly imprinted
- multiple sclerosis
- metabolic syndrome
- diabetic rats
- drug induced
- adverse drug
- preterm birth
- positron emission tomography