Current issues involving screening and identification of chemical contaminants in foods by mass spectrometry

Although quantitative analytical methods must be empirically validated prior to their use in a variety of applications, including regulatory monitoring of chemical adulterants in foods, validation of qualitative method performance for the analytes and matrices of interest is frequently ignored, or general guidelines are assumed to be true for specific situations. Just as in the case of quantitative method validation, acceptable method performance criteria should be established for qualitative analysis purposes to suit the analytical needs for given applications, and empirical method validation should be conducted to demonstrate the qualitative performance capabilities the method. This critical review article is intended to describe and discuss recent developments with of respect to qualitative aspects in mass spectrometry, and to make recommendations for validation of qualitative methods that meet common needs for monitoring of chemical contaminants in foods.

[1]  K. Speer,et al.  Analysis of triazole-based metabolites in plant materials using differential mobility spectrometry to improve LC/MS/MS selectivity. , 2012, Journal of AOAC International.

[2]  S. Uhlig,et al.  Assessment of detection methods in trace analysis by means of a statistically based in-house validation concept , 1998 .

[3]  Aviv Amirav,et al.  Open Probe fast GC–MS—Real time analysis with separation , 2014 .

[4]  V. Bartkevičs,et al.  Ultra high performance liquid chromatography-time-of-flight high resolution mass spectrometry in the analysis of hexabromocyclododecane diastereomers: method development and comparative evaluation versus ultra high performance liquid chromatography coupled to Orbitrap high resolution mass spectromet , 2014, Journal of chromatography. A.

[5]  Oliver Fiehn,et al.  Seven Golden Rules for heuristic filtering of molecular formulas obtained by accurate mass spectrometry , 2007, BMC Bioinformatics.

[6]  Thomas Kraemer,et al.  Liquid chromatography, in combination with a quadrupole time-of-flight instrument (LC QTOF), with sequential window acquisition of all theoretical fragment-ion spectra (SWATH) acquisition: systematic studies on its use for screenings in clinical and forensic toxicology and comparison with informatio , 2014, Analytical chemistry.

[7]  T. Delatour,et al.  Quantitative determination of four nitrofuran metabolites in meat by isotope dilution liquid chromatography-electrospray ionisation-tandem mass spectrometry. , 2005, Journal of chromatography. A.

[8]  Sergio C. Nanita,et al.  Ammonium chloride salting out extraction/cleanup for trace-level quantitative analysis in food and biological matrices by flow injection tandem mass spectrometry. , 2013, Analytica chimica acta.

[9]  P. Fodor,et al.  Routine approach to qualitatively screening 300 pesticides and quantification of those frequently detected in fruit and vegetables using liquid chromatography tandem mass spectrometry (LC-MS/MS) , 2010, Food additives & contaminants. Part A, Chemistry, analysis, control, exposure & risk assessment.

[10]  Clinton A. Krueger,et al.  High-performance ion mobility spectrometry with direct electrospray ionization (ESI-HPIMS) for the detection of additives and contaminants in food. , 2013, Analytica chimica acta.

[11]  M. Nielen,et al.  The Assessment of Selectivity in Different Quadrupole-Orbitrap Mass Spectrometry Acquisition Modes , 2015, Journal of The American Society for Mass Spectrometry.

[12]  A. Kaufmann,et al.  Correlation of precursor and product ions in single-stage high resolution mass spectrometry. A tool for detecting diagnostic ions and improving the precursor elemental composition elucidation. , 2013, Analytica chimica acta.

[13]  Tania Portolés,et al.  Screening of pesticides and polycyclic aromatic hydrocarbons in feeds and fish tissues by gas chromatography coupled to high-resolution mass spectrometry using atmospheric pressure chemical ionization. , 2014, Journal of agricultural and food chemistry.

[14]  J. Harnly,et al.  Probability of identification: a statistical model for the validation of qualitative botanical identification methods. , 2012, Journal of AOAC International.

[15]  J. V. Sancho,et al.  Validation of a qualitative screening method for pesticides in fruits and vegetables by gas chromatography quadrupole-time of flight mass spectrometry with atmospheric pressure chemical ionization. , 2014, Analytica chimica acta.

[16]  A. Gordin,et al.  Classical electron ionization mass spectra in gas chromatography/mass spectrometry with supersonic molecular beams. , 2008, Rapid communications in mass spectrometry : RCM.

[17]  M. Westphall,et al.  Development of a GC/Quadrupole-Orbitrap Mass Spectrometer, Part II: New Approaches for Discovery Metabolomics , 2014, Analytical chemistry.

[18]  Sergio C. Nanita,et al.  High-throughput pesticide residue quantitative analysis achieved by tandem mass spectrometry with automated flow injection. , 2009, Analytical chemistry.

[19]  A Kaufmann,et al.  Comprehensive comparison of liquid chromatography selectivity as provided by two types of liquid chromatography detectors (high resolution mass spectrometry and tandem mass spectrometry): "where is the crossover point?". , 2010, Analytica chimica acta.

[20]  H. Mol,et al.  Full scan MS in comprehensive qualitative and quantitative residue analysis in food and feed matrices: How much resolving power is required? , 2009 .

[21]  Rosa Pilolli,et al.  Orbitrap™ monostage MS versus hybrid linear ion trap MS: application to multi-allergen screening in wine. , 2014, Journal of mass spectrometry : JMS.

[22]  A. Kaufmann,et al.  Combining UHPLC and high-resolution MS: A viable approach for the analysis of complex samples? , 2014 .

[23]  Arjen Lommen Ultrafast PubChem searching combined with improved filtering rules for elemental composition analysis. , 2014, Analytical chemistry.

[24]  Oliver Fiehn,et al.  Metabolomic database annotations via query of elemental compositions: Mass accuracy is insufficient even at less than 1 ppm , 2006, BMC Bioinformatics.

[25]  H G J Mol,et al.  Guidelines for the validation of qualitative multi-residue methods used to detect pesticides in food. , 2012, Drug testing and analysis.

[26]  H. Mol,et al.  Identification in residue analysis based on liquid chromatography with tandem mass spectrometry: Experimental evidence to update performance criteria. , 2015, Analytica chimica acta.

[27]  M Farré,et al.  Application of ultra-high pressure liquid chromatography linear ion-trap orbitrap to qualitative and quantitative assessment of pesticide residues. , 2014, Journal of chromatography. A.

[28]  A. Kaufmann Strategy for the elucidation of elemental compositions of trace analytes based on a mass resolution of 100,000 full width at half maximum. , 2010, Rapid communications in mass spectrometry : RCM.

[29]  A Kaufmann,et al.  Development of an improved high resolution mass spectrometry based multi-residue method for veterinary drugs in various food matrices. , 2011, Analytica chimica acta.

[30]  L. Stolker,et al.  Trends in the identification of organic residues and contaminants: EC regulations under revision , 2001 .

[31]  Roy Macarthur,et al.  A protocol for the validation of qualitative methods of detection , 2012 .

[32]  A. Kaufmann,et al.  Post-run target screening strategy for ultra high performance liquid chromatography coupled to Orbitrap based veterinary drug residue analysis in animal urine. , 2013, Journal of chromatography. A.

[33]  Sergio C. Nanita,et al.  Fast extraction and dilution flow injection mass spectrometry method for quantitative chemical residue screening in food. , 2011, Journal of agricultural and food chemistry.

[34]  K. Giles,et al.  Are liquid chromatography/electrospray tandem quadrupole fragmentation ratios unequivocal confirmation criteria? , 2009, Rapid communications in mass spectrometry : RCM.

[35]  A. Kaufmann,et al.  Quantitative and confirmative performance of liquid chromatography coupled to high-resolution mass spectrometry compared to tandem mass spectrometry. , 2011, Rapid communications in mass spectrometry : RCM.

[36]  Anastasios Economou,et al.  Current mass spectrometry strategies for the analysis of pesticides and their metabolites in food and water matrices. , 2010, Mass spectrometry reviews.

[37]  Yu Bai,et al.  Applications of ambient mass spectrometry in high-throughput screening. , 2013, The Analyst.

[38]  J. Loco,et al.  Calculation of the decision limit (CCalpha) and the detection capability (CCbeta) for banned substances: the imperfect marriage between the quantitative and the qualitative criteria. , 2007, Analytica chimica acta.

[39]  Callee M. Walsh,et al.  Direct analysis of drugs in forensic applications using laser ablation electrospray ionization-tandem mass spectrometry (LAESI-MS/MS) , 2014 .

[40]  Imma Ferrer,et al.  Analysis of 100 pharmaceuticals and their degradates in water samples by liquid chromatography/quadrupole time-of-flight mass spectrometry. , 2012, Journal of chromatography. A.

[41]  B. Le Bizec,et al.  Comparative study of low- versus high-resolution liquid chromatography-mass spectrometric strategies for measuring perfluorinated contaminants in fish , 2011, Food additives & contaminants. Part A, Chemistry, analysis, control, exposure & risk assessment.

[42]  Sergio C. Nanita High-throughput chemical residue analysis by fast extraction and dilution flow injection mass spectrometry. , 2011, The Analyst.

[43]  A. Kaufmann,et al.  Evaluation of the interrelationship between mass resolving power and mass error tolerances for targeted bioanalysis using liquid chromatography coupled to high-resolution mass spectrometry. , 2013, Rapid communications in mass spectrometry : RCM.

[44]  F. Fernández,et al.  Ambient sampling/ionization mass spectrometry: applications and current trends. , 2011, Analytical chemistry.

[45]  Steven J Lehotay,et al.  Ruggedness testing and validation of a practical analytical method for >100 veterinary drug residues in bovine muscle by ultrahigh performance liquid chromatography-tandem mass spectrometry. , 2012, Journal of chromatography. A.

[46]  M. Holčapek,et al.  Recent developments in liquid chromatography-mass spectrometry and related techniques. , 2012, Journal of chromatography. A.

[47]  R. Subramanian,et al.  Comparison of information-dependent acquisition, SWATH, and MS(All) techniques in metabolite identification study employing ultrahigh-performance liquid chromatography-quadrupole time-of-flight mass spectrometry. , 2014, Analytical chemistry.

[48]  L. Stolker,et al.  The (Un)Certainty of Selectivity in Liquid Chromatography Tandem Mass Spectrometry , 2012, Journal of The American Society for Mass Spectrometry.

[49]  H. Mol,et al.  Qualitative aspects in the analysis of pesticide residues in fruits and vegetables using fast, low-pressure gas chromatography-time-of-flight mass spectrometry. , 2011, Journal of agricultural and food chemistry.

[50]  H. Mol,et al.  Validation of automated library-based qualitative screening of pesticides by comprehensive two-dimensional gas chromatography/time-of-flight mass spectrometry. , 2011, Journal of AOAC International.

[51]  S. Stein,et al.  Establishing the fitness for purpose of mass spectrometric methods , 2003, Journal of the American Society for Mass Spectrometry.

[52]  J A Sphon,et al.  Use of mass spectrometry for confirmation of animal drug residues. , 1978, Journal - Association of Official Analytical Chemists.

[53]  Jentaie Shiea,et al.  Ambient ionization mass spectrometry: a tutorial. , 2011, Analytica chimica acta.

[54]  Wanderson Romão,et al.  Ambient mass spectrometry: bringing MS into the “real world” , 2010, Analytical and bioanalytical chemistry.

[55]  Aviv Amirav,et al.  Gas chromatography-mass spectrometry with supersonic molecular beams. , 2008, Journal of mass spectrometry : JMS.

[56]  Sergio Armenta,et al.  A review of recent, unconventional applications of ion mobility spectrometry (IMS). , 2011, Analytica chimica acta.

[57]  Steven J Lehotay,et al.  Sampling and sample processing in pesticide residue analysis. , 2015, Journal of agricultural and food chemistry.

[58]  A. Kaufmann,et al.  Signal suppression can bias selected reaction monitoring ratios. Implications for the confirmation of positive findings in residue testing. , 2014, Rapid communications in mass spectrometry : RCM.

[59]  Brian Musselman,et al.  Evaluating a direct swabbing method for screening pesticides on fruit and vegetable surfaces using direct analysis in real time (DART) coupled to an Exactive benchtop orbitrap mass spectrometer , 2012, Analytical and Bioanalytical Chemistry.

[60]  Amadeo R Fernández-Alba,et al.  Issues in mass spectrometry between bench chemists and regulatory laboratory managers: summary of the roundtable on mass spectrometry held at the 123rd AOAC International Annual Meeting. , 2010, Journal of AOAC International.

[61]  T. Cajka,et al.  Challenging applications offered by direct analysis in real time (DART) in food-quality and safety analysis , 2011 .

[62]  A. Kaufmann,et al.  The current role of high-resolution mass spectrometry in food analysis , 2012, Analytical and Bioanalytical Chemistry.

[63]  N. Kuhnert,et al.  Investigation of isomeric flavanol structures in black tea thearubigins using ultraperformance liquid chromatography coupled to hybrid quadrupole/ion mobility/time of flight mass spectrometry. , 2014, Journal of mass spectrometry : JMS.

[64]  S. Kern,et al.  Accurate Mass Fragment Library for Rapid Analysis of Pesticides on Produce Using Ambient Pressure Desorption Ionization with High-Resolution Mass Spectrometry , 2014, Journal of The American Society for Mass Spectrometry.

[65]  Nandkishor S. Chindarkar,et al.  Liquid chromatography high-resolution TOF analysis: investigation of MSE for broad-spectrum drug screening. , 2014, Clinical chemistry.

[66]  S. Lehotay,et al.  Validation of a streamlined multiclass, multiresidue method for determination of veterinary drug residues in bovine muscle by liquid chromatography–tandem mass spectrometry , 2015, Analytical and Bioanalytical Chemistry.

[67]  H. Mol,et al.  Rapid detection of pesticides not amenable to multi-residue methods by flow injection–tandem mass spectrometry , 2014, Analytical and Bioanalytical Chemistry.

[68]  M. Nielen,et al.  Full-scan accurate mass selectivity of ultra-performance liquid chromatography combined with time-of-flight and orbitrap mass spectrometry in hormone and veterinary drug residue analysis , 2009, Journal of the American Society for Mass Spectrometry.

[69]  Sergio C. Nanita Quantitative mass spectrometry independence from matrix effects and detector saturation achieved by flow injection analysis with real-time infinite dilution. , 2013, Analytical chemistry.

[70]  W. Schwack,et al.  Planar solid phase extraction clean-up and microliter-flow injection analysis-time-of-flight mass spectrometry for multi-residue screening of pesticides in food. , 2014, Journal of chromatography. A.

[71]  T. V. van Beek,et al.  Macroscopic and microscopic spatially-resolved analysis of food contaminants and constituents using laser-ablation electrospray ionization mass spectrometry imaging , 2014, Analytical and Bioanalytical Chemistry.

[72]  A. Nuñez,et al.  Rapid analysis of aminoglycoside antibiotics in bovine tissues using disposable pipette extraction and ultrahigh performance liquid chromatography-tandem mass spectrometry. , 2013, Journal of chromatography. A.

[73]  A. Fernández-Alba,et al.  Laboratory assessment by combined z score values in proficiency tests: experience gained through the European Union proficiency tests for pesticide residues in fruits and vegetables , 2010, Analytical and bioanalytical chemistry.

[74]  Tania Portolés,et al.  Gas chromatography coupled to high-resolution time-of-flight mass spectrometry to analyze trace-level organic compounds in the environment, food safety and toxicology , 2011 .

[75]  E. Verdon,et al.  Evaluation of the limit of performance of an analytical method based on a statistical calculation of its critical concentrations according to ISO standard 11843: Application to routine control of banned veterinary drug residues in food according to European Decision 657/2002/EC , 2006 .

[76]  H. Mol,et al.  Qualitative aspects and validation of a screening method for pesticides in vegetables and fruits based on liquid chromatography coupled to full scan high resolution (Orbitrap) mass spectrometry , 2012, Analytical and Bioanalytical Chemistry.

[77]  L. Vanhaecke,et al.  High resolution Orbitrap mass spectrometry in comparison with tandem mass spectrometry for confirmation of anabolic steroids in meat. , 2013, Analytica chimica acta.

[78]  A. Kaufmann,et al.  Study of high-resolution mass spectrometry technology as a replacement for tandem mass spectrometry in the field of quantitative pesticide residue analysis. , 2012, Journal of AOAC International.

[79]  J. Lohne,et al.  Challenges in implementing a screening method for veterinary drugs in milk using liquid chromatography quadrupole time-of-flight mass spectrometry. , 2014, Journal of agricultural and food chemistry.

[80]  A. Kaufmann,et al.  Reliability of veterinary drug residue confirmation: high resolution mass spectrometry versus tandem mass spectrometry. , 2015, Analytica chimica acta.

[81]  Terry J. Dutko,et al.  Development and validation of a streamlined method designed to detect residues of 62 veterinary drugs in bovine kidney using ultra-high performance liquid chromatography--tandem mass spectrometry. , 2012, Drug testing and analysis.

[82]  Lukáš Václavík,et al.  Targeted analysis of multiple pharmaceuticals, plant toxins and other secondary metabolites in herbal dietary supplements by ultra-high performance liquid chromatography-quadrupole-orbital ion trap mass spectrometry. , 2014, Analytica chimica acta.

[83]  Zheng Ouyang,et al.  Ambient Mass Spectrometry , 2006, Science.

[84]  A. Kaufmann,et al.  Semi-targeted residue screening in complex matrices with liquid chromatography coupled to high resolution mass spectrometry: current possibilities and limitations. , 2011, The Analyst.

[85]  A. Kaufmann,et al.  False-positive liquid chromatography/tandem mass spectrometric confirmation of sebuthylazine residues using the identification points system according to EU directive 2002/657/EC due to a biogenic insecticide in tarragon. , 2009, Rapid communications in mass spectrometry : RCM.

[86]  B. Gamble,et al.  Surface swabbing technique for the rapid screening for pesticides using ambient pressure desorption ionization with high-resolution mass spectrometry. , 2011, Rapid communications in mass spectrometry : RCM.

[87]  Steven J. Lehotay,et al.  Sensitivity and noise in GC-MS: Achieving low limits of detection for difficult analytes , 2007 .

[88]  Steven J. Lehotay,et al.  Identification and confirmation of chemical residues in food by chromatography-mass spectrometry and other techniques , 2008 .

[89]  B. Chowdhry,et al.  Ion mobility spectrometry-mass spectrometry (IMS-MS) of small molecules: separating and assigning structures to ions. , 2013, Mass spectrometry reviews.

[90]  Jon W Wong,et al.  Ultrahigh-performance liquid chromatography electrospray ionization Q-Orbitrap mass spectrometry for the analysis of 451 pesticide residues in fruits and vegetables: method development and validation. , 2014, Journal of agricultural and food chemistry.

[91]  A. Fernández-Alba,et al.  Liquid chromatography-high-resolution mass spectrometry for pesticide residue analysis in fruit and vegetables: screening and quantitative studies. , 2013, Journal of chromatography. A.