Integration of Chemical Derivatization and in-Source Fragmentation Mass Spectrometry for High-Coverage Profiling of Submetabolomes
| Autor: | Cai-Feng Xiong, Na An, Yan-Zhen Wang, Yu-Qi Feng, Yu-Ning Hu, Quan-Fei Zhu |
|---|---|
| Rok vydání: | 2021 |
| Předmět: |
Profiling (computer programming)
Spectrometry Mass Electrospray Ionization Chromatography Analytical technique Carboxylic Acids Ms analysis High coverage Mass spectrometry Ion source Analytical Chemistry Mice chemistry.chemical_compound Fragmentation (mass spectrometry) chemistry Animals Derivatization Chromatography High Pressure Liquid Chromatography Liquid |
| Zdroj: | Analytical Chemistry. 93:11321-11328 |
| ISSN: | 1520-6882 0003-2700 |
| DOI: | 10.1021/acs.analchem.1c02673 |
| Popis: | In-source fragmentation-based high-resolution mass spectrometry (ISF-HRMS) is a potential analytical technique, which is usually used to profile some specific compounds that can generate diagnostic neutral loss (NL) or fragment ion (FI) in ion source inherently. However, the ISF-HRMS method does not work for those compounds that cannot inherently produce diagnostic NL or FI in ion source. In this study, a derivatization-based in-source fragmentation-information-dependent acquisition (DISF-IDA) strategy was proposed for profiling the metabolites with easily labeled functional groups (submetabolomes) by liquid chromatography-electrospray ionization-quadrupole time-of-flight mass spectrometry (LC-ESI-Q-TOF MS). As a proof-of-concept study, 36 carboxylated compounds labeled with N,N-dimethylethylenediamine (DMED) were selected as model compounds to examine performance of DISF-IDA strategy in screening the carboxylated metabolites and acquiring their MSn spectra. In ESI source, the DEMD-derived carboxylated compounds were fragmented to produce characteristic neutral losses of 45.0578, 63.0684, and/or 88.1000 Da that were further used as diagnostic features for screening the carboxylated metabolites by DISF-IDA-based LC-Q-TOF MS. Furthermore, high-resolution MSn spectra of the model compounds were also obtained within a single run of DISF-IDA-based LC-Q-TOF MS analysis, which contributed to the improvement of the annotation confidence. To further verify its applicability, DISF-IDA strategy was used for profiling carboxylated submetabolome in mice feces. Using this strategy, a total of 351 carboxylated metabolites were detected from mice feces, of which 178 metabolites (51% of the total) were positively or putatively identified. Moreover, DISF-IDA strategy was also demonstrated to be applicable for profiling other submetabolomes with easily labeled functional groups such as amino, carbonyl, and cis-diol groups. Overall, our proposed DISF-IDA strategy is a promising technique for high-coverage profiling of submetabolomes with easily labeled functional groups in biological samples. |
| Databáze: | OpenAIRE |
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