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Mass Spectral Filtering by Mass-Remainder Analysis (MARA) at High Resolution and Its Application to Metabolite Profiling of Flavonoids

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Mass Spectral Filtering by Mass-Remainder Analysis (MARA) at High Resolution and Its Application to Metabolite Profiling of Flavonoids International Journal of Molecular Sciences Article Mass Spectral Filtering by Mass-Remainder Analysis (MARA) at High Resolution and Its Application to Metabolite Profiling of Flavonoids Tibor Nagy 1 , Gerg˝oRóth 1,2, Ákos Kuki 1, Miklós Zsuga 1 and Sándor Kéki 1,* 1 Department of Applied Chemistry, Faculty of Science and Technology, University of Debrecen, Egyetem tér 1, H-4032 Debrecen, Hungary; [email protected] (T.N.); [email protected] (G.R.); [email protected] (Á.K.); [email protected] (M.Z.) 2 Doctoral School of Chemistry, University of Debrecen, Egyetem tér 1, H-4032 Debrecen, Hungary * Correspondence: [email protected]; Fax: +36-52-518662 Abstract: Flavonoids represent an important class of secondary metabolites because of their potential health benefits and functions in plants. We propose a novel method for the comprehensive flavonoid filtering and screening based on direct infusion mass spectrometry (DIMS) analysis. The recently invented data mining procedure, the multi-step mass-remainder analysis (M-MARA) technique is applied for the effective mass spectral filtering of the peak rich spectra of natural herb extracts. In addition, our flavonoid-filtering algorithm facilitates the determination of the elemental composition. M-MARA flavonoid-filtering uses simple mathematical and logical operations and thus, it can easily be implemented in a regular spreadsheet software. A huge benefit of our method is the high speed and the low demand for computing power and memory that enables the real time application even for tandem mass spectrometric analysis. Our novel method was applied for the electrospray ionization (ESI) DIMS spectra of various herb extract, and the filtered mass spectral data were subjected to chemometrics analysis using principal component analysis (PCA). Citation: Nagy, T.; Róth, G.; Kuki, Á.; Keywords: metabolomics; flavonoid; direct infusion mass spectrometry; mass spectral filtering; Zsuga, M.; Kéki, S. Mass Spectral Filtering by Mass-Remainder mass-remainder analysis; principal component analysis Analysis (MARA) at High Resolution and Its Application to Metabolite Profiling of Flavonoids. Int. J. Mol. Sci. 2021, 22, 864. https://doi.org/ 1. Introduction 10.3390/ijms22020864 Metabolomics is a comprehensive analysis that reveals the metabolome, i.e., all the metabolites of a biological system under study [1]. Metabolomics plays an increasingly Received: 27 December 2020 important role in plant science [2]. In metabolic analysis different analytical approaches Accepted: 14 January 2021 have been designed on several levels, such as “metabolite fingerprinting”, “metabolite Published: 16 January 2021 profiling”, and “metabolite target analysis” [1,3]. Metabolic profiling focuses on the analysis of a group of metabolites or a class of compounds. An important class of plant metabolites Publisher’s Note: MDPI stays neu- is the flavonoids because of their potential health benefits and functions in plants [4]. tral with regard to jurisdictional clai- Nearly 20,000 different flavonoids have now been characterized [5], with many of them ms in published maps and institutio- showing interesting antioxidant, anti-inflammatory, anti-mutagenic and anti-carcinogenic nal affiliations. properties [6,7]. They are active contributors to the health benefit of foods and beverages of plant origin, such as fruits, vegetables, tea, cocoa, and wine. Flavonoids have a C6-C3-C6 (A, C, B ring) core structure and depending on the position of the linkage between the C Copyright: © 2021 by the authors. Li- and B rings they can be divided into classes, while based on the degree of oxidation and censee MDPI, Basel, Switzerland. saturation in the heterocyclic C-ring the flavonoids may be divided into several groups. This article is an open access article For example, flavones, flavonols, flavanones, flavanonols, flavanols. In addition, the huge distributed under the terms and con- diversity of flavonoids arises from the number and complexity of substituents and presence ditions of the Creative Commons At- of additional heterocyclic rings [6,7]. The structures of the main flavonoid groups are tribution (CC BY) license (https:// shown in Scheme1. creativecommons.org/licenses/by/ 4.0/). Int. J. Mol. Sci. 2021, 22, 864. https://doi.org/10.3390/ijms22020864 https://www.mdpi.com/journal/ijms Int. J. Mol. Sci. 2021, 22, 864 2 of 12 Int. J. Mol. Sci. 2021, 22, x FOR PEER REVIEW 2 of 12 O O OH Flavan Flavanol O Chalcone DBE:9 DBE:9 DBE:9 O O O OH OH O O Anthocyanin Flavanone Flavanonol DBE: 10.5 DBE: 10 DBE: 10 O O OH O O Flavone Flavonol DBE: 11 DBE: 11 SchemeScheme 1. 1.The The structures structures of of main main flavonoid flavonoid groups groups and and their their double double bond bond equivalent equivalent (DBE) (DBE) values. val- ues. The identification and quantification of flavonoids requires sophisticated, advanced analyticalThe identification techniques. Mass and spectrometryquantification (MS)of flavonoids and nuclear requires magnetic sophisticated, resonance advanced (NMR) spectroscopy,analytical techniques. especially Mass when spectrometry they are coupled (MS) toand chromatographic nuclear magnetic techniques, resonance partic-(NMR) ularlyspectroscopy, liquid chromatography especially when (LC),they are are coup theled two to leading chromatographic analytical techniques, methods used particu- for metaboliclarly liquid profiling chromatography of natural (LC), extracts. are the Significant two leading advances analytical in hyphenated methods used techniques for meta- (LC–MS,bolic profiling LC–NMR), of natural as well extracts. as in combined Significant MS/NMR advances methods, in hyphenated have occurred techniques over (LC– the lastMS, decades LC–NMR),[3,8– 12as]. wellOn theas in other combined hand, theMS/NMR mass accuracy methods, and have resolving occurred power over of the high last resolutiondecades [3,8–12]. mass spectrometry On the other (HRMS) hand, the has mass dramatically accuracy improved and resolving the detection power of and high iden- res- tificationolution mass of compounds spectrometry in complex(HRMS) has natural dramat samplesically improved and, therefore, the detection has increased and identi- the relevancefication of of compounds non-hyphenated in complex MS methods. naturalDirect samples infusion and, therefore, mass spectrometry has increased (DIMS) the canrele- significantlyvance of non-hyphenated increase the analytical MS methods. throughput Direct compared infusion tomass LC–MS spectrometry [3,13]. However, (DIMS) the can rapidsignificantly identification increase of hundredsthe analytical or thousands throughput of compared mass peaks to arising LC–MS in [3,13]. direct However, injection ofthe complexrapid identification natural samples of hundreds requires advancedor thousands data of mining mass peaks techniques. arising Mass in direct defect injection filtering of (MDF)complex of natural complex samples MS data requires has been advanced used for data selectively mining techniques. detecting Mass compound defect classesfiltering having(MDF) similar of complex mass MS defects data has (where been mass used defect for selectively is the difference detecting between compound a compound’s classes hav- exacting similar mass and mass its defects nominal (where mass). mass The MDF defect process is the difference can facilitate between the detection a compound’s of the target exact compoundsmass and its by nominal the selective mass). removal The MDF of all process ions that can fall facilitate outside the of detection the preset of filter the masstarget rangecompounds window by [14 the–17 selective]. However, removal if the aimof all is ions the comprehensive that fall outside analysis of the ofpreset the flavonoids filter mass inrange complex window natural [14–17]. samples, However, a wide if mass the aim defect is the window comprehensive should be analysis applied thatof the would flavo- likelynoids include in complex many natural false peaks. samples, The a flavonoids wide mass fall defect into thewindow mass defectshould segment be applied where that numerouswould likely possible include chemical many compositionsfalse peaks. The may flavonoids be valid [ 18fall]. into the mass defect segment whereBesides numerous the MDF possible process, chemical the Kendrick compositions Mass may Defect be (KMD)valid [18]. [19 ] and related meth- ods [20Besides–22] (Re-KMD) the MDF areprocess, applied the for Kendrick the analysis Mass of Defect complex (KMD) mass [19] spectra, and related however, methods it is not[20–22] widespread (Re-KMD) in metabolomics. are applied for the analysis of complex mass spectra, however, it is not widespreadRecently, in we metabolomics. have developed a data mining algorithm, called mass-remainder analysis (MARA)Recently, and its we improved have developed variant, multi-step a data mining mass-remainder algorithm, called analysis mass-remainder (M-MARA) for anal- the processingysis (MARA) and and assessment its improved of complex variant, mass multi-step spectra mass-remainder [23–27]. In this paper, analysis we (M-MARA) propose a novel method for the comprehensive filtering and screening of flavonoids in the DIMS for the processing and assessment of complex mass spectra [23–27]. In this paper, we pro- spectra of natural extracts. pose a novel method for the comprehensive filtering and screening of flavonoids in the DIMS spectra of natural extracts. Int. J. Mol. Sci. 2021, 22, 864 3 of 12 Int. J. Mol. Sci. 2021, 22, x FOR PEER REVIEW 3 of 12 2.
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