Ultra-Performance Liquid Chromatography-Ion Mobility Separation-Quadruple Time-of-Flight MS (UHPLC-IMS-QTOF MS) Metabolomics for Short-Term Biomarker Discovery of Orange Intake: A Randomized, Controlled Crossover Study

Abstract

<jats:p>A major problem with dietary assessments is their subjective nature. Untargeted metabolomics and new technologies can shed light on this issue and provide a more complete picture of dietary intake by measuring the profile of metabolites in biological samples. Oranges are one of the most consumed fruits in the world, and therefore one of the most studied for their properties. The aim of this work was the application of untargeted metabolomics approach with the novel combination of ion mobility separation coupled to high resolution mass spectrometry (IMS-HRMS) and study the advantages that this technique can bring to the area of dietary biomarker discovery, with the specific case of biomarkers associated with orange consumption (Citrus reticulata) in plasma samples taken during an acute intervention study (consisting of a randomized, controlled crossover trial in healthy individuals). A total of six markers of acute orange consumption, including betonicines and conjugated flavonoids, were identified with the experimental data and previous literature, demonstrating the advantages of ion mobility in the identification of dietary biomarkers and the benefits that an additional structural descriptor, as the collision cross section value (CCS), can provide in this area.</jats:p>

Revealing the differences in collision cross section values of small organic molecules acquired by different instrumental designs and prediction models

“…Ion mobility spectrometry (IMS) has demonstrated to be a powerful additional technique for compound identification within target, suspect and non-target screening studies in various research fields [1][2][3][4]. IMS allows a conformational separation of ions based on their gaseous mobility through a drift gas (e.g., N2 or He) under the influence of an electric field.…”

Ion Mobility-High-Resolution Mass Spectrometry (IM-HRMS) for the Analysis of Contaminants of Emerging Concern (CECs): Database Compilation and Application to Urine Samples

“…However, for the use of IM-MS data for compound identification, the compilation of comprehensive databases containing CCS values of the compounds of interest is essential. In the past, the focus of available databases was on endogenous compounds, such as peptides, glycans, lipids, and steroids, reflecting that omics-based studies in different fields, such as metabolomics, , lipidomics, , plantomics, or proteomics, have been the predominant recent application of IM-MS. Yet, interest in the use of IM-MS for the analysis of CECs is rising.…”

Chromatography hyphenated to high resolution mass spectrometry in untargeted metabolomics for investigation of food (bio)markers

“…HILIC is commonly used simultaneously with RPLC to obtain a complementary information on those polar compounds that RPLC cannot separate. As example, this combination has been applied for discovery of consumption biomarkers [36,64]. and to study the effects of different diets on health [65,66].…”

“…Thus, the visualization of only the products ions from a specific precursor is feasible, enhancing the purity of the MS 2 spectrum with the inherent benefits of DIA acquisitions regarding available MS/MS data for all future biomarkers. The potential of this technique has been recently evaluated for orange dietary biomarkers discovery [64] and implemented for comparison of different polar lipids extraction methods to be used in evaluation of botanical origin, with potatoes as a case of study [110]. In both studies, data processing was performed using Progenesis QI (Waters), a unique software, able of performing the processing of 4D data obtained with xC-IMS-HRMS instruments.…”