Infrared matrix-assisted laser desorption electrospray ionization (IR-MALDESI) mass spectrometry imaging analysis of endogenous metabolites in cherry tomatoes

Bagley, M. Caleb; Pace, Crystal L.; Ekelöf, Måns; Muddiman, David C.

doi:10.1039/d0an00818d

Cited by 24 publications

(17 citation statements)

References 56 publications

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“…During the analysis of cherry tomatoes performed earlier, 15 several key metabolites were discovered using the MSiCorrelation tool in MSiReader. 48 MSiCorrelation does not rely on a database for identification, but rather returns the m/z signals that have similar abundance distributions to a reference m/z of interest.…”

Section: Resultsmentioning

confidence: 99%

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Investigations of β‐carotene radical cation formation in infrared matrix‐assisted laser desorption electrospray ionization (IR‐MALDESI)

Bagley

Muddiman

2021

Rapid Comm Mass Spectrometry

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Radical cationization of endogenous hydrocarbons in cherry tomatoes was previously reported using infrared matrix-assisted laser desorption electrospray ionization (IR-MALDESI), a mass spectrometry imaging technique that operates at ambient conditions and requires no sample derivatization. Due to the surprising nature of this odd-electron ionization, subsequent experiments were performed on β-carotene to determine the amount of radical cationization across different sampling conditions.Methods: β-Carotene was analyzed across a variety of sample states using IR-MALDESI followed by Orbitrap mass spectrometric analysis: first, as a standard in ethanol in a well plate; second, as particulates on printer paper; and third, as particulates covered by an ice matrix. These techniques were also performed with a β-carotene standard either in solution with a reducing agent (ascorbic acid) or with ascorbic acid in the electrospray solution.Results: Tandem mass spectrometry confirmed the presence of the radical cation of β-carotene by comparing fragments against NIST and METLIN databases. It was always analyzed as a radical cation when sampled from solution, where ascorbic acid increased radical cation abundance when in solution with β-carotene. Mixed-mode ionization between radical cationization and proton adduction was observed from dried particulates using IR-MALDESI.Conclusions: There are several potential mechanisms for β-carotene radical cationization prior to IR-MALDESI analysis, with multiphoton ionization, thermal degradation, and/or reaction with oxygen appearing to be the most logical explanations. Furthermore, although not the primary cause, changing certain aspects of sample conditions can result in significant mixed-mode ionization with competing protonation.

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Section: Resultsmentioning

confidence: 99%

“…14 Due to the post-desorption ESI of IR-MALDESI, most analytes are observed as protonated and sodiated species and other such even-electron ions. However, during a recent IR-MALDESI analysis of tomatoes, 15 the radical cationization of carotenoids was observed, ostensibly the first time for the technique.…”

Section: Introductionmentioning

confidence: 99%

Investigations of β‐carotene radical cation formation in infrared matrix‐assisted laser desorption electrospray ionization (IR‐MALDESI)

Bagley

Muddiman

2021

Rapid Comm Mass Spectrometry

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“…The study also found that the phenolic content of the cherry tomatoes per unit weight is 3–4 times greater than reported values for large-sized tomatoes and that lycopene showed strong activity against cervical carcinoma and lung cancer cells. Bagley et al [ 19 ] carried out a metabolomic analysis of commercial cherry tomatoes using infrared matrix-assisted laser desorption electrospray ionization (IR-M ALDESI) mass spectrometry imaging analysis. The results revealed the presence of 1626 unique compounds that included new cyanogenic glycosides, glucosinolates, and lignans.…”

Section: Discussionmentioning

confidence: 99%

Anti-Parasitic Activity of Cherry Tomato Peel Powders

Friedman

Tam

Kim

et al. 2021

Foods

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Trichomoniasis in humans, caused by the protozoal parasite Trichomonas vaginalis, is the most common non-viral sexually transmitted disease, while Tritrichomonas foetus causes trichomonosis, an infection of the gastrointestinal tract and diarrhea in farm animals and domesticated cats. As part of an effort to determine the inhibitory effects of plant-based extracts and pure compounds, seven commercially available cherry tomato varieties were hand-peeled, freeze-dried, and pounded into powders. The anti-trichomonad inhibitory activities of these peel powders at 0.02% concentration determined using an in vitro cell assay varied widely from 0.0% to 66.7% against T. vaginalis G3 (human); from 0.9% to 66.8% for T. foetus C1 (feline); and from 0.0% to 81.3% for T. foetus D1 (bovine). The organic Solanum lycopersicum var. cerasiforme (D) peels were the most active against all three trichomonads, inhibiting 52.2% (G3), 66.8% (C1), and 81.3% (D1). Additional assays showed that none of the powders inhibited the growth of foodborne pathogenic bacteria, pathogenic fungi, or non-pathogenic lactobacilli. Tomato peel and pomace powders with high content of described biologically active compounds could serve as functional food and feed additives that might help overcome adverse effects of wide-ranging diseases and complement the treatment of parasites with the anti-trichomonad drug metronidazole.

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“… 163 Agtuca et al explored the metabolic asymmetry between infected and noninfected soybean nodules with LAESI where elevated fatty acid, purine, and lipid levels occurred as a result of Bradyrhizobium japonicum infection. 164 The Muddiman group used ice matrices to increase lipid yields, 165 explored dynamic neurotransmitter imaging, 166 used IR-MALDESI for imaging metabolomics in plant and mammalian samples, 167 , 168 and coupled a drift tube for ion mobility direct collision cross section (CCS) measurements from several tissue types. 169 Most recently, cell-to-cell lipid heterogeneity in a dispersed HeLa cell culture was demonstrated by Xing et al with IR-MALDESI.…”

Section: Advances In Single-cell Ms Analysesmentioning

confidence: 99%

Spatially Resolved Mass Spectrometry at the Single Cell: Recent Innovations in Proteomics and Metabolomics

Taylor

Lukowski

Anderton

2021

J. Am. Soc. Mass Spectrom.

196

153

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Biological systems are composed of heterogeneous populations of cells that intercommunicate to form a functional living tissue. Biological function varies greatly across populations of cells, as each single cell has a unique transcriptome, proteome, and metabolome that translates to functional differences within single species and across kingdoms. Over the past decade, substantial advancements in our ability to characterize omic profiles on a single cell level have occurred, including in multiple spectroscopic and mass spectrometry (MS)-based techniques. Of these technologies, spatially resolved mass spectrometry approaches, including mass spectrometry imaging (MSI), have shown the most progress for single cell proteomics and metabolomics. For example, reporter-based methods using heavy metal tags have allowed for targeted MS investigation of the proteome at the subcellular level, and development of technologies such as laser ablation electrospray ionization mass spectrometry (LAESI-MS) now mean that dynamic metabolomics can be performed in situ. In this Perspective, we showcase advancements in single cell spatial metabolomics and proteomics over the past decade and highlight important aspects related to high-throughput screening, data analysis, and more which are vital to the success of achieving proteomic and metabolomic profiling at the single cell scale. Finally, using this broad literature summary, we provide a perspective on how the next decade may unfold in the area of single cell MS-based proteomics and metabolomics.

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Infrared matrix-assisted laser desorption electrospray ionization (IR-MALDESI) mass spectrometry imaging analysis of endogenous metabolites in cherry tomatoes

Abstract: We report the spatially resolved metabolic profiling of cherry tomatoes using infrared matrix-assisted laser desorption electrospray ionization (IR-MALDESI); an ambient mass spectrometry imaging (MSI) technique that requires no sample derivatization.

Cited by 24 publications

References 56 publications

Investigations of β‐carotene radical cation formation in infrared matrix‐assisted laser desorption electrospray ionization (IR‐MALDESI)

Investigations of β‐carotene radical cation formation in infrared matrix‐assisted laser desorption electrospray ionization (IR‐MALDESI)

Anti-Parasitic Activity of Cherry Tomato Peel Powders

Spatially Resolved Mass Spectrometry at the Single Cell: Recent Innovations in Proteomics and Metabolomics

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