DOCSLIB.ORG

MARA): an Improved Method for Elemental Composition Assignment in Petroleomics

Total Page：16

File Type：pdf, Size：1020Kb

Download full-text PDF Read full-text
MARA): an Improved Method for Elemental Composition Assignment in Petroleomics View metadata, citation and similar papers at core.ac.uk brought to you by CORE provided by University of Debrecen Electronic Archive Subscriber access provided by UNIV OF LOUISIANA Article Mass-Remainder Analysis (MARA): An Improved Method for Elemental Composition Assignment in Petroleomics. Tibor Nagy, Ákos Kuki, Miklós Nagy, Miklos Zsuga, and Sándor Kéki Anal. Chem., Just Accepted Manuscript • Publication Date (Web): 26 Mar 2019 Downloaded from http://pubs.acs.org on March 30, 2019 Just Accepted “Just Accepted” manuscripts have been peer-reviewed and accepted for publication. They are posted online prior to technical editing, formatting for publication and author proofing. The American Chemical Society provides “Just Accepted” as a service to the research community to expedite the dissemination of scientific material as soon as possible after acceptance. “Just Accepted” manuscripts appear in full in PDF format accompanied by an HTML abstract. “Just Accepted” manuscripts have been fully peer reviewed, but should not be considered the official version of record. They are citable by the Digital Object Identifier (DOI®). “Just Accepted” is an optional service offered to authors. Therefore, the “Just Accepted” Web site may not include all articles that will be published in the journal. After a manuscript is technically edited and formatted, it will be removed from the “Just Accepted” Web site and published as an ASAP article. Note that technical editing may introduce minor changes to the manuscript text and/or graphics which could affect content, and all legal disclaimers and ethical guidelines that apply to the journal pertain. ACS cannot be held responsible for errors or consequences arising from the use of information contained in these “Just Accepted” manuscripts. is published by the American Chemical Society. 1155 Sixteenth Street N.W., Washington, DC 20036 Published by American Chemical Society. Copyright © American Chemical Society. However, no copyright claim is made to original U.S. Government works, or works produced by employees of any Commonwealth realm Crown government in the course of their duties. Page 1 of 8 Analytical Chemistry 1 2 3 4 5 6 7 Mass-Remainder Analysis (MARA): An Improved Method for 8 Elemental Composition Assignment in Petroleomics. 9 10 Tibor Nagy, Ákos Kuki, Miklós Nagy, Miklós Zsuga, Sándor Kéki* 11 12 Department of Applied Chemistry, Faculty of Science and Technology, University of Debrecen, H-4032 Debrecen, Egyetem 13 tér 1., Hungary 14 ABSTRACT: Data processing and visualization methods have an important role in the mass spectrometric study of crude oils and 15 other natural samples. The recently invented data mining procedure: the Mass-remainder analysis (MARA), was further developed 16 for the use in petroleomics. MARA is based on the calculation of the remainder after dividing by the exact mass of a base unit, in 17 petroleomics by the mass of the CH2 group. The two key steps in the MARA algorithm are the separation of the monoisotopic 18 peaks from the other isotopic peaks and the subsequent intensity correction. The effectiveness of our MARA method was 19 demonstrated on the analysis of lubricating mineral oil and crude oil samples by ultra-high resolution Fourier transform ion 20 cyclotron resonance mass spectrometry (FT-ICR-MS) experiments. MARA is able to handle a huge portion of the overlapped peaks 21 even in a moderate resolution mass spectrum. Using MARA, effective chemical composition assignment and visual representation 22 were achieved for complex mass spectra recorded by a TOF analyzer with a limited resolution of 40 000 at m/z 400. In the absence of an ultra-high resolution mass analyzer, MARA can provide a closer look on the mass spectral peaks, like a digital zoom in a 23 simple camera. 24 25 26 + + 27 type (e.g. both the [C30H54OS + H] and [C30H57O3N3 + H] ions Introduction 28 have almost the same KMD values 0.120619 and 0.120468, 29 Crude oil is a very complex mixture of hydrocarbons and polar respectively). In order to differentiate between the above compositions, a better than 0.2 ppm mass accuracy is required at 30 organic compounds. As the world’s remaining oil reserves are becoming heavier and sourer, the knowledge of the molecular m/z 400. During the mass peak assignation, this issue can be 31 composition of crude oil is ever more important. The mass eliminated by pre-sorting the compounds according to their 32 spectrometric analysis of this extremely complex mixture may nominal mass (the mass peaks are divided into 14 nominal mass 33 require ultrahigh mass resolution and mass measurement accuracy series), as proposed by Hsu et al.24, however these coincidences 34 to separate the tens of thousands of individual compounds present are still interfering during the visualization and in the filtering 35 in crude oil. Fourier transform ion cyclotron resonance mass based on the KMD plots. Recently we have proposed a simple 36 spectrometry (FT-ICR-MS) has been successfully applied for algorithm, the Mass-remainder analysis (MARA) for the crude oil characterization.1-10. As alternatives, the performance of processing of complex copolymer mass spectra.26 MARA can not 37 “zig-zag” multi-reflecting time-of-flight (TOF) analyzer with only handle the issues mentioned above, but does not require a 38 ultrahigh resolving power,11 and Orbitrap Fourier transform mass multiple sorting algorithm. In this work, we demonstrate the 39 spectrometer were also used for petroleomic studies.12 ability of the Mass-remainder analysis for the elemental 40 Independently of analysers, fractionation of the sample is composition assignment and subsequent intensity correction by 41 beneficial, especially for non-polar compounds.13-15 The SARA the analysis of lubricating mineral oil and crude oil samples 42 (saturates, aromatics, resins, asphaltenes) fractionation is typical recorded FT-ICR-MS experiments. Moreover, owing to its for crude oil, and the collection of subfractions can increase the deisotoping procedure, MARA is expected to be able to analyze 43 number of assignations.16-19 Beside the identification of the the complex crude oil mass spectra recorded by a TOF analyzer 44 chemical composition, the structural analysis allows a better with moderate resolving power. With MARA, we report a new 45 understanding of crude oil behavior.20,21 Not only the high way for the data processing in petroleomics, and furthermore, to 46 resolution and mass accuracy, but also the data processing and the best of our knowledge, there have been no studies on the 47 visualization methods, such as Kendrick mass defect22 and van characterization of crude oil by a TOF analyzer with limited 23 48 Krevelen analyses have an important role in the study of crude resolution (40 000 at m/z 400). oils. Kendrick suggested a new mass scale, which converts the 49 mass of CH from 14.01565 to an integer value of 14. The Experimental 50 2 Kendrick mass defect (KMD) plot provides a tool for the sorting Chemicals. The crude oil sample is originated from Russia, 51 of compounds into homologous series. KMD plot simplifies the imported by the MOL group (Budapest, Hungary). LVO 100 1,2,24 52 identification of the mass peaks or enables the rapid lubricant oil (free of additives) was produced by Leybold (Vienna, 53 characterization of the sample by filtering characteristic Austria). Unused and used LVO 100 lubricants were measured. 25 54 compound classes. The compounds containing the same The used LVO 100 was applied in a rotary vacuum pump for 6 55 heteroatoms O, N and S (same class) and the number of rings plus months. Methanol (HPLC grade) and acetic acid (100%, double bonds (same type) but different numbers of CH groups 56 2 analytical reagent) were purchased from VWR International will have the same KMD values. Unfortunately, the Kendrick (Leuven, Belgium). Toluene was received from Sigma-Aldrich 57 mass defect calculations can generate coincidences, namely (Taufkirchen, Germany) and distilled before use. The samples 58 identical KMD values for the compounds of different class and/or 59 60 ACS Paragon Plus Environment Analytical Chemistry Page 2 of 8 were dissolved in toluene and completed with methanol. samples probably contain mass peak pairs m/z1 and m/z2 with m/z2 1 Concentration of the samples were 1.5 mg/mL, the solvent was - m/z1 = n R/round(R) + ε differences, where R = 14.01565, 2 toluene methanol mixture (V/V 4:1). 1 mL of the samples were round(R) = 14, n is an integer and ε (and ε' in Eq. 3) are small 3 spiked by 3 μL acetic acid and prepared freshly before each values. 4 measurement. For the comparison of FT-ICR and TOF measurements the concentration was 0.1 mg/mL. 5 Electrospray Quadrupole Time-of-Flight Mass 6 Spectrometry (ESI-QTOF MS). A Maxis II type Qq-TOF MS 7 instrument (Bruker Daltonik, Bremen, Germany) was used 8 equipped with an electrospray ion source where the spray voltage 9 was 4.5 kV. The resolution of the instrument is 40 000 at m/z 400 10 (FWHM), the mass accuracy is <600 ppb (internal calibration). N2 11 was utilized as drying (200°C, 4.0 L/min) and nebulizer gas (0.5 12 bar). The mass spectra were recorded by means of a digitizer at a sampling rate of 2 GHz. The spectra were calibrated in two steps, 13 externally by ESI tune mix (first step), from Bruker, and + 14 internally using [CnH2n-13N+H] (DBE = 8) well known series 15 appeared with high intensity (second step). The spectra were 16 evaluated with the Compass DataAnalysis 4.4 software from 17 Bruker. The sample solutions were introduced directly into the 18 ESI source with a syringe pump (Cole-Parmer Ins.
Load more

Recommended publications
  • And Ion Mobility – Mass Spectrometry As Platforms for X-Omic Analyses
    ABSTRACT Fueling Advances in Ultra Performance Liquid Chromatography – and Ion Mobility – Mass Spectrometry as Platforms for X-omic Analyses Sharon Michelle Munisamy, Ph.D. Mentor: C. Kevin Chambliss, Ph.D. Analysis of x-omics samples presents a significant challenge to analytical chemists. The complexity and diversity of x-omics samples make it difficult to determine or develop the right analytical approach. This dissertation presents novel applications of ultra performance liquid chromatography – high-resolution mass spectrometry (UPLC- HRMS) and ion mobility – high-resolution mass spectrometry (IM-HRMS) in two emerging x-omics areas: lignocellulomics and petroleomics. Compared to traditional methods of x-omics analyses, these techniques offer higher chromatographic efficiency with UPLC, which can equate to faster analysis times and greater separation, an additional degree of separation with ion mobility spectrometry (IMS), and high peak resolution and mass accuracy with HRMS, which allow for identification of known and unknown analytes. Direct infusion electrospray ionization – ion mobility – high-resolution mass spectrometry (DIESI-IM-HRMS) has been evaluated as a rapid technique for the determination of total molecular composition in “whole-sample” biomass hydrolysates and extracts. IM-HRMS data reveal a high molecular weight range of biomass components (up to 1100 m/z) and provide trendline isolation of feedstock components from those introduced “in process”. Carbohydrates and other lignocellulosic degradation products were identified via HRMS exact mass measurements (with typical mass errors less than 5 ppm). Analyte assignments were supported via IM-MS collision-cross-section (CCS) measurements and trendline analysis. An automated “omics” approach utilizing UPLC-HR-TOF-MS was developed for the identification of previously unknown lignocellulosic degradation products.
    [Show full text]
  • Mass Spectrometry Analysis and Raw Data Processing
    molecules Review Characterization of Lignin Compounds at the Molecular Level: Mass Spectrometry Analysis and Raw Data Processing Ruochun Zhang 1,2, Yulin Qi 1,2,*, Chao Ma 1, Jinfeng Ge 1, Qiaozhuan Hu 1, Fu-Jun Yue 1,2 , Si-Liang Li 1,2 and Dietrich A. Volmer 3 1 Institute of Surface-Earth System Science, School of Earth System Science, Tianjin University, Tianjin 300072, China; [email protected] (R.Z.); [email protected] (C.M.); [email protected] (J.G.); [email protected] (Q.H.); [email protected] (F.-J.Y.); [email protected] (S.-L.L.) 2 Tianjin Key Laboratory of Earth Critical Zone Science and Sustainable Development in Bohai Rim, Tianjin University, Tianjin 300072, China 3 Department of Chemistry, Humboldt-Universität zu Berlin, 12489 Berlin, Germany; [email protected] * Correspondence: [email protected]; Fax: +86-022-27405051 Abstract: Lignin is the second most abundant natural biopolymer, which is a potential alternative to conventional fossil fuels. It is also a promising material for the recovery of valuable chemicals such as aromatic compounds as well as an important biomarker for terrestrial organic matter. Lignin is currently produced in large quantities as a by-product of chemical pulping and cellulosic ethanol processes. Consequently, analytical methods are required to assess the content of valuable chemicals contained in these complex lignin wastes. This review is devoted to the application of mass spec- trometry, including data analysis strategies, for the elemental and structural elucidation of lignin products. We describe and critically evaluate how these methods have contributed to progress and trends in the utilization of lignin in chemical synthesis, materials, energy, and geochemistry.
    [Show full text]
  • 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).
    [Show full text]
  • 63-67 3번 Sunghwan Kim(Reveiw)
    Vol. 3, No. 3, 2012 REVIEW www.msletters.org | Mass Spectrometry Letters Data Interpretation Methods for Petroleomics Annana Islama, Yunju Choa, Arif Ahmeda, and Sunghwan Kima,b* aKyungpook National University, Department of Chemistry, Daegu, 702-701, Korea bGreen-Nano Materials Research Center, Daegu, 702-701, Korea Received September 4, 2012; Revised September 12, 2012; Accepted September 12, 2012 First published on the web September 20, 2012; DOI: 10.5478/MSL.2012.3.3.63 I. Introduction ...................................................................................................................... 63 II. Kendrick mass defect plot ............................................................................................... 64 III. Van Krevelen diagram ...................................................................................................... 64 IV. Double-bond equivalence vs. carbon number plot ......................................................... 65 V. Application of statistical analysis .................................................................................... 66 VI. Correlation analysis ......................................................................................................... 66 VII. Conclusions and future studies ........................................................................................ 67 VIII. Acknowledgement ...........................................................................................................67 IX. References .......................................................................................................................
    [Show full text]
  • Selective Ionisation and Affordable High Resolution Mass Spectrometry Is Revolutionising Molecular Characterisation in the Petroleum and Petrochemical Industries
    SELECTIVE IONISATION AND AFFORDABLE HIGH RESOLUTION MASS SPECTROMETRY IS REVOLUTIONISING MOLECULAR CHARACTERISATION IN THE PETROLEUM AND PETROCHEMICAL INDUSTRIES Since its early days High Resolution Mass Spectrometry (HRMS) has been a key technique for the molecular characterisation of the complex mixtures experienced in the petroleum based industries and in recent years the power and application of the technique has increased dramatically. Author Tom Lynch In 2005 Marshall and Rogers (1)(2) wrote “Ultrahigh-resolution Fourier transform ion cyclotron resonance mass spectrometry has recently revealed that petroleum crude oil contains heteroatom- containing (N,O,S) organic components having more than 20 000 distinct elemental compositions. It is therefore now possible to contemplate the ultimate characterisation of all of the chemical constituents of petroleum, along with their interactions and reactivity, a concept we denote as “Petroleomics”. Selective resolution of the components of interest is the key to successfully analysing complex sample matrices by any technique and in mass spectrometry this can be achieved by a combination of the resolution of the mass analyser with selective ionisation which targets only the compound classes of interest. In addition, the components of interest can be resolved from matrix interferences by coupling with pre-separation techniques such chromatography or ion mobility spectrometry. In Rodgers and McKenna’s (3) review of Petroleum Analysis in 2011 more than half the text discussed advances in mass spectrometry with the remainder covering all other analytical techniques. This dominance was attributed to developments in a range of atmospheric pressure ionisation techniques combined with the resolving power of Fourier Transform Ion Cyclotron Resonance Mass Spectrometers (FT- ICR-MS).
    [Show full text]
  • Simulated Ageing of Crude Oil and Advanced Oxidation Processes for Water Remediation Since Crude Oil Pollution
    catalysts Article Simulated Ageing of Crude Oil and Advanced Oxidation Processes for Water Remediation since Crude Oil Pollution Filomena Lelario 1, Giuliana Bianco 1 , Sabino Aurelio Bufo 1,2,* and Laura Scrano 3 1 Department of Sciences, University of Basilicata, Via dell’Ateneo Lucano 10, 85100 Potenza, Italy; fi[email protected] (F.L.); [email protected] (G.B.) 2 Department of Geography, Environmental Management & Energy Studies, University of Johannesburg, Johannesburg 2092, South Africa 3 Department of European Cultures (DICEM), University of Basilicata, 75100 Matera, Italy; [email protected] * Correspondence: [email protected]; Tel.: +39-0971-6237 Abstract: Crude oil can undergo biotic and abiotic transformation processes in the environment. This article deals with the fate of an Italian crude oil under simulated solar irradiation to understand (i) the modification induced on its composition by artificial ageing and (ii) the transformations arising from different advanced oxidation processes (AOPs) applied as oil-polluted water remediation methods. The AOPs adopted were photocatalysis, sonolysis and, simultaneously, photocatalysis and sonolysis (sonophotocatalysis). Crude oil and its water-soluble fractions underwent analysis using GC-MS, liquid-state 1H-NMR, Fourier transform ion cyclotron resonance mass spectrometry (FT-ICR-MS), and fluorescence. The crude oil after light irradiation showed (i) significant modifications induced by the artificial ageing on its composition and (ii) the formation of potentially toxic substances. The treatment produced oil oxidation with a particular effect of double bonds oxygenation. Non-polar compounds present in the water-soluble oil fraction showed a strong presence of branched alkanes Citation: Lelario, F.; Bianco, G.; Bufo, S.A.; Scrano, L.
    [Show full text]
  • Ultrahigh Resolution Mass Spectrometry: Determining the Molecular Composition of Petroleum
    26 Analytical Instrumentation Ultrahigh Resolution Mass Spectrometry: Determining the Molecular Composition of Petroleum Dr. Mark P. Barrow University of Warwick, Coventry CV4 7AL, UK E-Mail: [email protected] Fourier transform ion cyclotron resonance mass spectrometry (FTICR MS) has been at the forefront of petroleum analysis for more than a decade. Not to be confused with Fourier transform infrared (FTIR) spectroscopy, FTICR MS represents the state-of-the-art for mass spectrometry. The performance characteristics and fl exibility of the instrumentation have made the technique extremely well-suited to the analysis of complex mixtures, such as petroleum and environmental samples. Introduction to FTICR MS where f is the cyclotron frequency in hertz (Hz), q is the charge on the ion in coulombs (C), B is the magnetic fl ux density in tesla (T), and m is the mass of the ion in kilograms (kg). Note that m/z can First described in 1974 by Comisarow and Marshall,1 the underlying principle is that ions are trapped be determined by converting the mass from units of kg to daltons (Da) and through the relationship by appropriate electric and magnetic fi elds,2-4 orbiting within a “cell.” The cell is typically a cylinder shown in Equation (2): of a few centimetres in diameter, consisting of six electrodes: two, circular end plates (trapping electrodes) and four electrodes spanning the length of the cylinder (two detection electrodes and (2) two excitation electrodes). The cell is located within a magnetic fi eld, most commonly positioned within the bore of a superconducting magnet.
    [Show full text]
  • Kendrick Mass Defect Approach Combined to NORINE Database for Molecular Formula Assignment of Nonribosomal Peptides
    B American Society for Mass Spectrometry, 2019 J. Am. Soc. Mass Spectrom. (2019) 30:2608Y2616 DOI: 10.1007/s13361-019-02314-3 RESEARCH ARTICLE Kendrick Mass Defect Approach Combined to NORINE Database for Molecular Formula Assignment of Nonribosomal Peptides Mickaël Chevalier,1 Emma Ricart,2 Emeline Hanozin,3 Maude Pupin,4,5 Philippe Jacques,6 Nicolas Smargiasso,3 Edwin De Pauw,3 Frédérique Lisacek,2 Valérie Leclère,1 Christophe Flahaut1 1Univ. Lille, INRA, ISA, Univ. Artois, Univ. Littoral Côte d’Opale, EA 7394-Institut Charles Viollette (ICV), F-59000, Lille, France 2Proteome informatics Group, SIB Swiss Institute of Bioinformatics (SIB), and Computer Science Department, University of Geneva, Geneva, Switzerland 3Mass Spectrometry Laboratory, Molecular Systems - MolSys Research Unit, University of Liège, Liège, Belgium 4Univ. Lille, CNRS, Centrale Lille, UMR 9189 - CRIStAL - Centre de Recherche en Informatique Signal et Automatique de Lille, F-59000, Lille, France 5Inria-Lille Nord Europe, Bonsai team, F-59655, Villeneuve d’Ascq Cedex, France 6TERRA Research Centre, Microbial Processes and Interactions (MiPI), Gembloux Agro-Bio Tech University of Liège, B-5030, Gembloux, Belgium Abstract. The identification of known (dereplication) or unknown nonribosomal pep- tides (NRPs) produced by microorganisms is a time consuming, expensive, and challenging task where mass spectrometry and nuclear magnetic resonance play a key role. The first step of the identification process always involves the estab- lishment of a molecular formula. Unfortunately, the number of potential molecular formulae in- creases significantly with higher molecular masses and the lower precision of their measurements. In the present article, we demonstrate that molecular formula assignment can be achieved by a combined approach using the regular Kendrick mass defect (RKMD) and NORINE, the reference curated database of NRPs.
    [Show full text]
  • Going Beyond the Analysis of Common
    Florida International University FIU Digital Commons FIU Electronic Theses and Dissertations University Graduate School 11-14-2016 Going Beyond the Analysis of Common Contaminants: Target, Suspect, and Non-Target Analysis of Complex Environmental Matrices by High-Resolution Mass Spectrometry Anna Katarina Huba Florida International University, [email protected] DOI: 10.25148/etd.FIDC001186 Follow this and additional works at: https://digitalcommons.fiu.edu/etd Part of the Analytical Chemistry Commons, and the Environmental Chemistry Commons Recommended Citation Huba, Anna Katarina, "Going Beyond the Analysis of Common Contaminants: Target, Suspect, and Non-Target Analysis of Complex Environmental Matrices by High-Resolution Mass Spectrometry" (2016). FIU Electronic Theses and Dissertations. 3048. https://digitalcommons.fiu.edu/etd/3048 This work is brought to you for free and open access by the University Graduate School at FIU Digital Commons. It has been accepted for inclusion in FIU Electronic Theses and Dissertations by an authorized administrator of FIU Digital Commons. For more information, please contact [email protected]. FLORIDA INTERNATIONAL UNIVERSITY Miami, Florida GOING BEYOND THE ANALYSIS OF COMMON CONTAMINANTS: TARGET, SUSPECT, AND NON-TARGET ANALYSIS OF COMPLEX ENVIRONMENTAL MATRICES BY HIGH-RESOLUTION MASS SPECTROMETRY A dissertation submitted in partial fulfillment of the requirements for the degree of DOCTOR OF PHILOSOPHY in CHEMISTRY by Anna Katarina Huba 2016 ! To: Dean Michael R. Heithaus College of Arts, Sciences and Education This dissertation, written by Anna Katarina Huba, and entitled Going Beyond the Analysis of Common Contaminants: Target, Suspect, and Non-Target Analysis of Complex Environmental Matrices by High-Resolution Mass Spectrometry, having been approved in respect to style and intellectual content, is referred to you for judgment.
    [Show full text]
  • Using Mass Spectrometry As a Reaction Detector
    bioRxiv preprint doi: https://doi.org/10.1101/855148; this version posted June 14, 2020. The copyright holder for this preprint (which was not certified by peer review) is the author/funder. All rights reserved. No reuse allowed without permission. 1 Reactomics: using mass spectrometry as a 2 reaction detector 3 4 Miao Yu1, Lauren Petrick1,2* 5 1 Department of Environmental Medicine and Public Health, Icahn School of Medicine at Mount 6 Sinai, New York, NY, 10029, United States 7 2 Institute for Exposomic Research, Icahn School of Medicine at Mount Sinai, New York, NY, 8 10029, United States 9 *Corresponding author: Email: [email protected] Phone: +1-212-241-7351. Fax: +1- 10 646-537-9654. 11 bioRxiv preprint doi: https://doi.org/10.1101/855148; this version posted June 14, 2020. The copyright holder for this preprint (which was not certified by peer review) is the author/funder. All rights reserved. No reuse allowed without permission. 12 13 Abstract 14 15 Untargeted metabolomics analysis captures chemical reactions among small molecules. Common 16 mass spectrometry-based metabolomics workflows first identify the small molecules 17 significantly associated with the outcome of interest, then begin exploring their biochemical 18 relationships to understand biological fate (environmental studies) or biological impact 19 (physiological response). We suggest an alternative by which biochemical relationships can be 20 directly retrieved through untargeted high-resolution paired mass distance (PMD) analysis 21 without a priori knowledge of the identities of participating compounds. Retrieval is done using 22 high resolution mass spectrometry as a chemical reaction detector, where PMDs calculated from 23 the mass spectrometry data are linked to biochemical reactions obtained via data mining of small 24 molecule and reaction databases, i.e.
    [Show full text]
  • An Efficient Data Filtering Strategy for Easy Metabolite Detection from the Direct Analysis of a Biological Fluid Using Fourier Transform Mass Spectrometry
    An efficient data filtering strategy for easy metabolite detection from the direct analysis of a biological fluid using Fourier transform mass spectrometry Estelle Rathahao, Sandra Alves, Laurent Debrauwer, Jean Pierre Cravedi, Alain Paris To cite this version: Estelle Rathahao, Sandra Alves, Laurent Debrauwer, Jean Pierre Cravedi, Alain Paris. An efficient data filtering strategy for easy metabolite detection from the direct analysis of a biological fluidusing Fourier transform mass spectrometry. Rapid Communications in Mass Spectrometry, Wiley, 2017, 31 (6), pp.485-494. 10.1002/rcm.7812. hal-01594553 HAL Id: hal-01594553 https://hal.archives-ouvertes.fr/hal-01594553 Submitted on 26 Sep 2017 HAL is a multi-disciplinary open access L’archive ouverte pluridisciplinaire HAL, est archive for the deposit and dissemination of sci- destinée au dépôt et à la diffusion de documents entific research documents, whether they are pub- scientifiques de niveau recherche, publiés ou non, lished or not. The documents may come from émanant des établissements d’enseignement et de teaching and research institutions in France or recherche français ou étrangers, des laboratoires abroad, or from public or private research centers. publics ou privés. An efficient data filtering strategy for easy metabolite detection from the direct analysis of a biological fluid using Fourier transform mass spectrometry Estelle Rathahao-Paris1,*, Sandra Alves2, Laurent Debrauwer3,4, Jean-Pierre Cravedi3 and Alain Paris5 1 UMR Ingénierie Procédés Aliments, AgroParisTech, Inra, Université Paris-Saclay, 91300 Massy, France; 2 Sorbonne Universités, Université Pierre et Marie Curie, Institut Parisien de Chimie Moléculaire, UMR8232, 4 Place Jussieu, 75252 Paris, France; 3 Toxalim, Université de Toulouse, INRA, INP-ENVT, INP-EI-Purpan, Univ.
    [Show full text]
  • A High-Resolution Mass Spectrometer to Measure Atmospheric Ion Composition
    Atmos. Meas. Tech., 3, 1039–1053, 2010 www.atmos-meas-tech.net/3/1039/2010/ Atmospheric doi:10.5194/amt-3-1039-2010 Measurement © Author(s) 2010. CC Attribution 3.0 License. Techniques A high-resolution mass spectrometer to measure atmospheric ion composition H. Junninen1, M. Ehn1, T. Petaj¨ a¨1, L. Luosujarvi¨ 2, T. Kotiaho2,3, R. Kostiainen3, U. Rohner4, M. Gonin4, K. Fuhrer4, M. Kulmala1, and D. R. Worsnop1,5 1Department of Physics, P.O. Box 64, 00014, University of Helsinki, Helsinki, Finland 2Department of Chemistry, P.O. Box 55, 00014, University of Helsinki, Helsinki, Finland 3Division of Pharmaceutical Chemistry, P.O. Box 56, 00014, University of Helsinki, Helsinki, Finland 4Tofwerk AG, 3600 Thun, Switzerland 5Aerodyne Research Inc, Billerica, MA 01821, USA Received: 24 December 2009 – Published in Atmos. Meas. Tech. Discuss.: 12 February 2010 Revised: 14 July 2010 – Accepted: 18 July 2010 – Published: 17 August 2010 Abstract. In this paper we present recent achievements acids and their clusters. The positive ions were more com- on developing and testing a tool to detect the composition plex, the main compounds were (poly)alkyl pyridines and – of ambient ions in the mass/charge range up to 2000 Th. amines. The APi-TOF provides a near universal interface for The instrument is an Atmospheric Pressure Interface Time- atmospheric pressure sampling, and this key feature will be of-Flight Mass Spectrometer (APi-TOF, Tofwerk AG). Its utilized in future laboratory and field studies. mass accuracy is better than 0.002%, and the mass resolv- ing power is 3000 Th/Th. In the data analysis, a new effi- cient Matlab based set of programs (tofTools) were devel- 1 Introduction oped, tested and used.
    [Show full text]