Novel Isotope-Coded Photochemical Derivatization Coupled with LC-MS and MS Imaging Platform Enables Sensitive Quantification and Accurate Localization of Amine Submetabolome in Pancreatic Disease

Analytical Chemistry, Journal Year: 2025, Volume and Issue: unknown

Published: March 17, 2025

Alterations in amine metabolite levels are closely associated with the poor progression of pancreatic disease, including acute pancreatitis (AP) and cancer (PC). However, effectively quantifying visualizing these metabolites through mass spectrometry (MS) has proven to be challenging. Here, we have designed a novel rapid strategy for analyzing submetabolome within liquid chromatography-mass (LC-MS) air-flow-assisted desorption electrospray ionization imaging (AFADESI-MSI) platforms by inducing pair isotope-labeling-based photochemical derivatization reagents. The simultaneous introduction 4-amino-1-methylpyridinium moiety renders 160- 1037-fold higher response MS. Coupled full MS-ddMS2 precursor ion scan modes, this labeling allows straightforward detection 423 peaks indazolone derivatives identification 82 biological samples. semiquantitation amines plasma from AP patients healthy controls resulted discovery unreported aromatic aminoaldehydes significant changes employing ethanolamine distinguishing severities early stage. In MSI platform, reagent can efficiently derivatize primary avoiding spatial deviation significantly enhancing sensitivity rat brain kidney. Further joint analysis pancreas PC use two allowed identifying metabolite, methylamine. These results together enhance role amine-driven biomarker diagnosis disease accelerate application on-tissue derivation MSI.

Language: Английский

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Sample preparation for fatty acid analysis in biological samples with mass spectrometry-based strategies

Analytical and Bioanalytical Chemistry, Journal Year: 2024, Volume and Issue: 416(9), P. 2371 - 2387

Published: Feb. 6, 2024

Language: Английский

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Stable Isotope Labeling-Based Nontargeted Strategy for Characterization of the In Vitro Metabolic Profile of a Novel Doping BPC-157 in Doping Control by UHPLC-HRMS

Molecules, Journal Year: 2023, Volume and Issue: 28(21), P. 7345 - 7345

Published: Oct. 30, 2023

Traditional strategies for the metabolic profiling of doping are limited by unpredictable pathways and numerous proportions background chemical noise that lead to inadequate metabolism knowledge, thereby affecting selection optimal detection targets. Thus, a stable isotope labeling-based nontargeted strategy combined with ultra-high-performance liquid chromatography-high-resolution mass spectrometry (UHPLC-HRMS) was first proposed effective rapid analysis small-molecule agents demonstrated via its application novel BPC-157. Using 13C/15N-labeled BPC-157, complete workflow including automatic 13C0,15N0-13C6,15N2m/z pair picking based on characteristic behaviors pairs constructed, one metabolite produced pathway plus eight metabolites conventional amide-bond breaking were successfully discovered from two incubation models. Furthermore, specific method BPC-157 five main in human urine developed validated satisfactory limits (0.01~0.11 ng/mL) excellent quantitative ability (linearity: 0.02~50 ng/mL R2 > 0.999; relative error (RE)% < 10% standard deviation (RSD)% 5%; recovery 90%). The vitro profile could provide new insights into biotransformation improved targets control.

Language: Английский

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Strategy to Empower Nontargeted Metabolomics by Triple-Dimensional Combinatorial Derivatization with MS-TDF Software

Analytical Chemistry, Journal Year: 2024, Volume and Issue: 96(19), P. 7634 - 7642

Published: May 1, 2024

Chemical derivatization is a widely employed strategy in metabolomics to enhance metabolite coverage by improving chromatographic behavior and increasing the ionization rates mass spectroscopy (MS). However, might complicate MS data, posing challenges for data mining due lack of corresponding benchmark database. To address this issue, we developed triple-dimensional combinatorial nontargeted metabolomics. This utilizes three structurally similar reagents supported MS-TDF software accelerated processing. Notably, simultaneous specific functional groups biological samples produced compounds with stable but distinct retention times numbers, facilitating discrimination MS-TDF, an in-house processing software. In study, carbonyl analogues human plasma were derivatized using combination hydrazide-based reagents: 2-hydrazinopyridine, 2-hydrazino-5-methylpyridine, 2-hydrazino-5-cyanopyridine (6-hydrazinonicotinonitrile). approach was applied identify potential biomarkers lung cancer. Analysis validation demonstrated that our improved recognition accuracy metabolites reduced risk false positives, providing useful method studies. The MATLAB code available on GitHub at https://github.com/CaixiaYuan/MS-TDF.

Language: Английский

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An Economically Viable Stable lsotope-Enhanced Multiple Reaction Monitoring Method for Total Fatty Acid Analysis in a Mouse odel of Non-Alcoholic Fatty Liver Disease

Journal of Chromatography A, Journal Year: 2024, Volume and Issue: 1736, P. 465406 - 465406

Published: Sept. 30, 2024

Language: Английский

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Comprehensive analysis of amino acid alterations during Candida albicans biofilm inhibition by Shikonin using non-targeted and stable isotope-labeled targeted metabolomics

Microchemical Journal, Journal Year: 2024, Volume and Issue: unknown, P. 112378 - 112378

Published: Dec. 1, 2024

Language: Английский

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