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Talanta

Talanta

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Bromine signature coded derivatization LC-MS for specific profiling of carboxyl or carbonyl-containing metabolites in Mycoplasma pneumoniae infection

Published:6 December 2024 DOI: 10.1016/j.talanta.2024.127345 PMID: 39673980
Jie Han,?Qinyan Yang,?Zheng Zhi,?Na Li,?Jian-Lin Wu

Abstract

Carboxyl or carbonyl-containing metabolites (CoCCMs) are widely distributed in biological samples. Global profiling of CoCCMs is essential for ascertaining specific functions of metabolites and their potential physiological roles in biogenic activities. However, simultaneous determination of these compounds is hampered by poor ionization efficiency, vast polarity differences, wide discrepancy of concentration ranges. Herein, a novel bromine isotope derivatization reagent 5-bromo-2- hydrazinopyridine was employed for CoCCMs profiling by liquid chromatography-mass spectrometry (LC-MS). This method enabled rapid derivatization of 44 CoCCMs under mild conditions. Enhanced separation efficiencies, detection sensitivities, and distinctive MS fragmentation characteristics were observed. Furthermore, this method was demonstrated to be efficient in revealing metabolic alternations, and abnormal serum levels of 6-keto-PGF1α, 12(S)-HHTrE, 15(S)-HEPE and N-acetyl tryptophan were disclosed for the first time in Mycoplasma pneumoniae (MP) infectious patients. Finally, based on the distinctive 2?Da differences of molecular ion peak pairs with almost 1:1 intensity ratio originated from 79Br and 81Br isotopes, an MS-DIAL and Python assisted MS1 isotope screening-MS2 fragments characterization combination strategy was developed for rapid screening, classification, and identification of detected CoCCMs. A total of 1069 CoCCMs were detected, of which 198 CoCCMs were identified in untargeted analysis. Statistical analysis revealed altered metabolic pathways, while glutamic acid, oxoglutaric acid, succinic acid, pyruvic acid, glyceric acid, and glycine were selected as potential biomarkers of MP infection. This bromine signature coded derivatization-LC-MS approach was proved to be a valuable tool for global probing of CoCCMs in biological samples with high sensitivity and broad coverage.

Substances (4)

Materials
Procduct Name CAS Molecular Formula Supplier Price
Ursodeoxycholic acid 128-13-2 C24H40O4 804 suppliers $30.00-$3418.80
HATU 148893-10-1 C10H15F6N6OP 689 suppliers $6.00-$2848.00
LITHOCHOLIC ACID 434-13-9 C24H40O3 392 suppliers $10.00-$427.00
5-BETA-CHOLANIC ACID-7-ALPHA, 12-ALPHA-DIOL 566-17-6 C24H40O4 34 suppliers $62.00-$2085.00