Multiclass screening of >200 pharmaceutical and other residues in aquatic foods by ultrahigh-performance liquid chromatography–quadrupole-Orbitrap mass spectrometry

AbstractA quick screening method of more than 200 pharmaceutical and other residues in aquatic foods based on ultrahigh-performance liquid chromatography–quadrupole-Orbitrap mass spectrometry (UHPLC-Q/Orbitrap MS) was established. In this method, after the addition of 200 μL of 1 M EDTA-Na2, 2 g of each sample homogenate was extracted successively with 10 mL of acetonitrile and 10 mL of ethyl acetate. The extracts were combined, dried under nitrogen flow, and redissolved in 0.1% formic acid in acetonitrile/water (4:6, v/v) for analysis. The prepared samples were analyzed by UHPLC- Q/Orbitrap MS system in Full MS/ddMS2 (full-scan data-dependent MS/MS) mode. Compound identification was performed through comparison of the sample data with the database for standard chemicals, including the retention time, precursor ion, product ions, and isotope pattern for all 206 compounds. Five different aquatic food matrices (carp, shrimp, crab, eel, and mussel) spiked with the analytes at 1, 10, and 50 ng/g were evaluated to assess recoveries, precision, matrix effects, stability, and detection limits using the method. UHPLC analyses required 25 min, and 178–200 analytes met identification criteria at 50 ng/g depending on the matrix. Furthermore, practical application of this method for real samples displayed strong screening capability. Graphical abstractA quick screening method of >200 pharmaceutical and other residues in aquatic foods based on ultrahighperformance liquid chromatography–quadrupole-Orbitrap mass spectrometer was established. Fivedifferent aquatic food matrices, including carp, shrimp, crab, eel and mussel, were studied to evaluatescreen limit at 1, 10 and 50 μg·kg-1 level. Results suggest the high reliability, high time-efficiency and goodsimplicity of the method.

[1]  Li Zhang,et al.  Rapid determination of 88 veterinary drug residues in milk using automated TurborFlow online clean-up mode coupled to liquid chromatography-tandem mass spectrometry. , 2016, Talanta.

[2]  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.

[3]  T. Rocha-Santos,et al.  Contaminants in aquaculture: Overview of analytical techniques for their determination , 2016 .

[4]  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.

[5]  X. Xia,et al.  Determination of nitrofurans metabolites residues in aquatic products by ultra-performance liquid chromatography-tandem mass spectrometry. , 2016, Food chemistry.

[6]  Bertrand Rochat,et al.  Proposed Confidence Scale and ID Score in the Identification of Known-Unknown Compounds Using High Resolution MS Data , 2017, Journal of The American Society for Mass Spectrometry.

[7]  Steven Morris,et al.  Distribution and fate of HBCD and TBBPA brominated flame retardants in North Sea estuaries and aquatic food webs. , 2004, Environmental science & technology.

[8]  Roberto Romero-González,et al.  Analysis of veterinary drug and pesticide residues in animal feed by high-resolution mass spectrometry: comparison between time-of-flight and Orbitrap , 2015, Food additives & contaminants. Part A, Chemistry, analysis, control, exposure & risk assessment.

[9]  Muhammet Raşit Sünbül,et al.  Organochlorine pesticide, antibiotic and heavy metal residues in mussel, crayfish and fish species from a reservoir on the Euphrates River, Turkey. , 2017, Environmental pollution.

[10]  Veit Schwämmle,et al.  High‐performance hybrid Orbitrap mass spectrometers for quantitative proteome analysis: Observations and implications , 2016, Proteomics.

[11]  Jinping Li,et al.  Multi-residue method for the determination of organofluorine pesticides in fish tissue by liquid chromatography triple quadrupole tandem mass spectrometry. , 2016, Food chemistry.

[12]  P. Teale,et al.  Capabilities and Limitations of High‐Resolution Mass Spectrometry (HRMS): Time‐of‐flight and Orbitrap™ , 2016 .

[13]  Thomas Letzel,et al.  Non-target screening with high-resolution mass spectrometry: critical review using a collaborative trial on water analysis , 2015, Analytical and Bioanalytical Chemistry.

[14]  Jian Wang,et al.  Development and Validation of a Multiclass Method for Analysis of Veterinary Drug Residues in Milk Using Ultrahigh Performance Liquid Chromatography Electrospray Ionization Quadrupole Orbitrap Mass Spectrometry. , 2015, Journal of agricultural and food chemistry.

[15]  Oscar Núñez,et al.  New trends in fast liquid chromatography for food and environmental analysis. , 2012, Journal of chromatography. A.

[16]  A. Gentili,et al.  Veterinary drugs residues: a review of the latest analytical research on sample preparation and LC-MS based methods , 2017, Food additives & contaminants. Part A, Chemistry, analysis, control, exposure & risk assessment.

[17]  Roberto Romero-González,et al.  Comprehensive analysis of toxics (pesticides, veterinary drugs and mycotoxins) in food by UHPLC-MS , 2014 .

[18]  Qiaoyuan Cheng,et al.  Application of ultra-high-performance liquid chromatography coupled with LTQ-Orbitrap mass spectrometry for identification, confirmation and quantitation of illegal adulterated weight-loss drugs in plant dietary supplements. , 2017, Journal of chromatography. B, Analytical technologies in the biomedical and life sciences.

[19]  Marilena E. Dasenaki,et al.  Qualitative Multiresidue Screening Method for 143 Veterinary Drugs and Pharmaceuticals in Milk and Fish Tissue Using Liquid Chromatography Quadrupole-Time-of-Flight Mass Spectrometry. , 2015, Journal of agricultural and food chemistry.

[20]  A. A. Abd El-Aty,et al.  Determination of fenobucarb residues in animal and aquatic food products using liquid chromatography-tandem mass spectrometry coupled with a QuEChERS extraction method. , 2017, Journal of chromatography. B, Analytical technologies in the biomedical and life sciences.

[21]  T. Nagata,et al.  Simultaneous Determination of Thiamphenicol, Florfenicol, and Chloramphenicol Residues in Muscles of Animals and Cultured Fish by Liquid Chromatography , 1992 .

[22]  Jianzhong Shen,et al.  Immunoassays for the detection of macrocyclic lactones in food matrices – A review , 2017 .

[23]  Albino Gallina,et al.  Development and validation of a QuEChERS method coupled to liquid chromatography and high resolution mass spectrometry to determine pyrrolizidine and tropane alkaloids in honey. , 2017, Food chemistry.

[24]  Jim E Riviere,et al.  Health concerns and management of select veterinary drug residues. , 2016, Food and chemical toxicology : an international journal published for the British Industrial Biological Research Association.

[25]  R. Cifelli,et al.  Analytical methods for the endocrine disruptor compounds determination in environmental water samples. , 2016, Journal of chromatography. A.

[26]  J. Lohne,et al.  Wide-Scope Screening Method for Multiclass Veterinary Drug Residues in Fish, Shrimp, and Eel Using Liquid Chromatography-Quadrupole High-Resolution Mass Spectrometry. , 2017, Journal of agricultural and food chemistry.

[27]  Carmen Cruces-Blanco,et al.  Determination of quinolones in fish by ultra-high performance liquid chromatography with fluorescence detection using QuEChERS as sample treatment , 2015 .

[28]  Feng Zhang,et al.  High-throughput untargeted screening of veterinary drug residues and metabolites in tilapia using high resolution orbitrap mass spectrometry. , 2017, Analytica chimica acta.

[29]  Yolanda Picó,et al.  Determination of pesticides and veterinary drug residues in food by liquid chromatography-mass spectrometry: A review. , 2016, Analytica chimica acta.

[30]  Nikolaos S Thomaidis,et al.  Multi-residue determination of 115 veterinary drugs and pharmaceutical residues in milk powder, butter, fish tissue and eggs using liquid chromatography-tandem mass spectrometry. , 2015, Analytica chimica acta.

[31]  A. Boxall,et al.  Assessment of the Risks of Mixtures of Major Use Veterinary Antibiotics in European Surface Waters. , 2016, Environmental science & technology.

[32]  J. Lohne,et al.  Review: Application of High Resolution Mass Spectrometry to Monitor Veterinary Drug Residues in Aquacultured Products. , 2015, Journal of AOAC International.

[33]  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.

[34]  T. Anumol,et al.  Comparison of veterinary drug residue results in animal tissues by ultrahigh-performance liquid chromatography coupled to triple quadrupole or quadrupole–time-of-flight tandem mass spectrometry after different sample preparation methods, including use of a commercial lipid removal product , 2017, Analytical and Bioanalytical Chemistry.

[35]  Edward I. Broughton,et al.  Policies and practices for aquaculture food safety in China , 2010 .

[36]  M. Scippo,et al.  Withdrawal time for sulfamethoxazole and trimethoprim following treatment of striped catfish (Pangasianodon hypophthalmus) and hybrid red tilapia (Oreochromis mossambicus × Oreochromis niloticus) , 2015 .