固相萃取-超高效液相色谱串联质谱法测定水产品中磺胺类药物残留
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摘要
目的建立同时测定水产品中磺胺嘧啶(sulfadiazine, SDZ)、磺胺甲恶唑(sulfamethoxazole, SMZ)、磺胺二甲嘧啶(sulfadimidine, SDM)、磺胺间甲氧嘧啶(sulfamonomethoxine, SMM)4种磺胺类药物残留的固相萃取-超高效液相色谱-串联质谱的检测方法。方法样品采用乙腈-0.2%甲酸溶液均质振荡提取,用CaptivaEMR-Lipid固相萃取柱净化,外标法定量。结果 4种磺胺类药物的检出限为0.08～0.12μg/kg,定量限为0.25～0.50μg/kg,回收率均为70.2%～103.4%之间。结论该方法具有基质干扰小、准确,易操作等优点,适用于水产品中4种磺胺类残留药物的检测。
Objective To establish a method for the determination of 4 kinds of sulfonamide drugs(sanodiazine,sulfamethoxazole, sulfadimidine and sulfamonomethoxine) residues in aquatic product by solid phase extraction-ultra performance liquid chromatography tandem mass spectrometry. Methods Samples were extracted with 0.2% formic acid acetonitrile solution, and the extract was purified on Captiva EMR–lipid solid phase extraction column. Quantification of the analytes was achieved by UPLC-MS using the external standard method. Results The results showed that the limits of detection(LODs) of 4 sulfonamide were in range of 0.08-0.12 μg/kg and the limits of quantification(LOQ) were in range of 0.25-0.50 μg/kg. The average recoveries of 4 sulfonamide drugs were from 70.2% to 103.4%. Conclusion This method has the advantages of low matrix interference, accuracy and easy operation, which is suitable for the detection of 4 kinds of sulfonamides residues in aquatic products.
Objective To establish a method for the determination of 4 kinds of sulfonamide drugs(sanodiazine,sulfamethoxazole, sulfadimidine and sulfamonomethoxine) residues in aquatic product by solid phase extraction-ultra performance liquid chromatography tandem mass spectrometry. Methods Samples were extracted with 0.2% formic acid acetonitrile solution, and the extract was purified on Captiva EMR–lipid solid phase extraction column. Quantification of the analytes was achieved by UPLC-MS using the external standard method. Results The results showed that the limits of detection(LODs) of 4 sulfonamide were in range of 0.08-0.12 μg/kg and the limits of quantification(LOQ) were in range of 0.25-0.50 μg/kg. The average recoveries of 4 sulfonamide drugs were from 70.2% to 103.4%. Conclusion This method has the advantages of low matrix interference, accuracy and easy operation, which is suitable for the detection of 4 kinds of sulfonamides residues in aquatic products.
引文
[1]吴永宁,邵兵,沈建忠.兽药残留检测与监控技术[M].北京:化学工业出版社,2007.Wu YN,Shao B,Shen JZ.The technology of detection and monitoring of veterinary drug residue[M].Beijing:Chemical Industry Press,2007.
[2]Codex Alimentarius Commission.Maximum residue limits(MRLs)and risk management recommendations(RMRs)for residue of veterinary drugs in foods:CAC/MRL 2-2015[S].
[3]中华人民共和国农业部.动物性食品中兽药最高残留限量:农业部235号公告[Z].2002-12-24.Ministry of Agriculture of the People,s Republic of China.MRLs in animal foods:Ministry of Agriculture No.235[Z].2002-12-24.
[4]中国兽药典委员会.中华人民共和国兽药典[M].北京:中国农业出版社,2010.China Veterinary Pharmacopoeia Committee.Veterinary pharmacopoeia of the PRC[M].Beijing:China Agriculture Press,2010.
[5]代婷婷,林华萍,段婕,等.毛细管区带电泳化学发光法测定食品中残留的磺胺类药物[J].分析化学,2016,(5):747-753.Dai TT,Lin HP,Duan J,et al.Determination of sulfonamides residues in food by capillary zone electrophoresis-chemiluminescence method[J].Chin J Anal Chem,2016,(5):747-753.
[6]Font G,Juangarcía A,PicóY.Pressurized liquid extraction combined with capillary electrophoresis-mass spectrometry as an improved methodology for the determination of sulfonamide residues in meat[J].J Chromatogr A,2007,1159(1-2):233-241.
[7]Zhou Q,Peng D,Wang Y,et al.A novel hapten and monoclonal-base d enzyme-linked immunosorbent assay for sulfonam ides in edible animal tissues[J].Food Chem,2014,(154):52-62.
[8]Peng D,Li Z,Wang Y,et al.Enzyme-linked immunoassay based on imprinted microspheres for the detection of sulfamethazine residue[J].JChromatogr A,2017,(1506):9-17.
[9]冯敏,李亚楠,高丼霞,等.酶联免疫吸附法在食品安全性指标检测中的研究迚展[J].食品安全质量检测学报,2016,7(10):3973-3979.Feng M,Li YN,Gao LX,et al.Research progress of enzyme-linked immunosorbent assay in food safety indices detection[J].J Food Saf Qual,2016,(10):3973-3979.
[10]田博,金坚,惠人杰,等.兽药残留检测中磺胺嘧啶ELISA试剂盒的研制[J].生物加工过程,2017,15(1):69-72.Tian B,Jin J,Hui RJ,et al.Determination of sulfadiazine in the veterinary drugs residue by sensitive ELISA[J].Chin J Bioprocess Eng,2017,15(1):69-72.
[11]苏明明,肖姗姗,张瑜,等.酶联免疫试剂盒检测牛血清中磺胺类药物残留[J].检验检疫学刊,2016,(2):17-19,30.Su MM,Xiao SS,Zhang Y,et al.The detection of sulfa drug residues using ELISA for bovine serum[J].J Inspect Quarant,2016,(2):17-19,30.
[12]李君华,米振杰,李志平,等.磺胺二甲嘧啶药物残留ELISA检测试剂盒的研制及初步应用[J].中国畜牧杂志,2013,(9):78-81.Li JH,Mi ZJ,Li ZP,et al.Development and preliminary application of ELISA kit for the detection of sulfamethazine residues[J]Chin J Anim Husband,2013,(9):78-81.
[13]罗贵昆,陈旭,谢体波,等.阿维菌素类药物酶联免疫快速检测试剂盒的制备及检测效果[J].中外食品工业,2014,(7):19-22.Luo GK,Chen X,Xie TB,et al.Preparation and effect of ELISA kit for rapid detection of abamectin[J].Global Food Ind,2014,(7):19-22.
[14]Ostermaier S,Schneider E,Usleber E,et al.Rapid enzyme immunoassays for the detection of three sulphonamides in milk[J].Food Agric Imunol,1995,7(3):253-258.
[15]张萍,陈燕,王晓玱.固相萃取-高效液相色谱法同时测定鸡蛋粉中12种磺胺类药物残留量药物[J].药物分析杂志,2010,30(12):2338-2343.Zhang P,Chen Y,Wang XL.Simultaneous determination of 12sulfonamide residues in egg powder by solid phase extraction and high performance liquid chromatography[J].J Pharm Anal,2010,30(12):2338-2343.
[16]陈吉之,闫超.饲料中9种磺胺类药物的HPLC法快速分离与检测[J].中国医药工业杂志,2015,6(8):892-894.Chen JZ,Yan C.Rapid separation and detection of 9 sulfonamides in feed by HPLC[J].Chin J Pharm Ind,2015,6(8):892-894.
[17]Zhang YP,Xu X,Qi X,et al.Determination of sulfonamides in livers using matix solid-phase dispersion extraction high-performance liquid chromatography[J].J Sparat Sci,2012,35(1):45-52.
[18]李雪德,鲜启明,刘红玱,等.高效液相色谱-荧光检测法同时测定蔬菜中3种磺胺类药物残留[J].分析化学,2010,38(3):429-433.Li XD,Xian QM,Liu HL,et al.Simultaneous determination of 3sulfonamides residues in vegetables by high performance liquid chromatography with fluorescence detection[J].Anal Chem,2010,38(3):429-433.
[19]吴翠琴,陈迪云,陈永亨,等.荧光胺衍生液相色谱法测定猪肝中10种磺胺[J].分析实验室,2018,37(12):1370-1374.Wu CQ,Chen DY,Chen YX,et al.Determination of 10 sulfonamides in pig liver by HPLC derived from fluorescein[J].Chin J Anal Lab,2018,37(12):1370-1374.
[20]王浩,启雷,殷晓燕,等.液相色谱-串联三重四极杆质谱对牛奶中10种磺胺类药物残留的同时测定[J].分析测试学报,2008,27(s):137-139.Wang H,Qi L,Yin XY,et al.Simultaneous determination of ten sulfonamides residues in mike by LC-MS/MS method[J].J Instrum Anal,2008,27(s):137-139.
[21]张晓强,张波,方萍,等.QuEChERS-超高效液相色谱-串联质谱法快速测定鱼肉中22种磺胺类药物残留[J].理化检验-化学分册,2015,51(3):369-374.Zhang XQ,Zhang B,Fang P,et al.Rapid determination of 22 sulfonamide residues in fish by QuEChERS-UPLC-MS/MS[J].Phys Test Chem Anal B,2015,51(3):369-374.
[22]Yu H,Tao YF,Chen DM,et al.Development of a high performance liquid chromatography method and a liquid chromatography-tandem mass spectrometry method with the pressurized liquid extraction for the quantification and confirmation of sulfonamides in the foods of animal origin[J].J Chromatogr B,2011,879(25):2653-2662.
[23]Heller DN,Ngoh MA,Donoghue D,et al.Identification of incurred sulfonamide residues in eggs:Methods for confirmation by liquid chromatography-tandem mass spectrometry and quantitation by liquid chromatography with ultraviolet detection[J].J Chromatogr B,2002,774(1):39-52.
[24]黄华,陈君慧,冯楠,等.动物源性食品中磺胺类药物残留前处理和检测方法研究迚展[J].食品工业科技,2013,34(4):378-381.Huang H,Chen JH,Feng N,et al.Research progress in the pre-processing and detection method of sulfonamides drugs residues in animal derived foods[J].Sci Technol Food Ind,2013,34(4):378-381.
[25]Pecorelli I,Bibi R,Fioroni L,et al.Validation of a confirmatory method for the determination of sulphonamides in muscle according to the European Union regulation 2002/657/EC[J].J Chromatogr A,2004,1032(1-2):23-29.
[26]Tso J,Agad S.A systematic investigation to optimize simultaneous extraction and liquid chromatography tandem mass spectrometry analysis of estrogens and their conjugated metabolites in milk[J].J Chromatogr A,2010,1217(29):4784-4795.
[27]Gomezperez ML,Romero-gonzalez R,Martinezvidal JL,et al.Analysis of veterinary drug residues in cheese by ultra-high-performance LC coupled to triple quadrupole MS/MS[J].J Sparat Si,2013,36(7):1223-1230.
[2]Codex Alimentarius Commission.Maximum residue limits(MRLs)and risk management recommendations(RMRs)for residue of veterinary drugs in foods:CAC/MRL 2-2015[S].
[3]中华人民共和国农业部.动物性食品中兽药最高残留限量:农业部235号公告[Z].2002-12-24.Ministry of Agriculture of the People,s Republic of China.MRLs in animal foods:Ministry of Agriculture No.235[Z].2002-12-24.
[4]中国兽药典委员会.中华人民共和国兽药典[M].北京:中国农业出版社,2010.China Veterinary Pharmacopoeia Committee.Veterinary pharmacopoeia of the PRC[M].Beijing:China Agriculture Press,2010.
[5]代婷婷,林华萍,段婕,等.毛细管区带电泳化学发光法测定食品中残留的磺胺类药物[J].分析化学,2016,(5):747-753.Dai TT,Lin HP,Duan J,et al.Determination of sulfonamides residues in food by capillary zone electrophoresis-chemiluminescence method[J].Chin J Anal Chem,2016,(5):747-753.
[6]Font G,Juangarcía A,PicóY.Pressurized liquid extraction combined with capillary electrophoresis-mass spectrometry as an improved methodology for the determination of sulfonamide residues in meat[J].J Chromatogr A,2007,1159(1-2):233-241.
[7]Zhou Q,Peng D,Wang Y,et al.A novel hapten and monoclonal-base d enzyme-linked immunosorbent assay for sulfonam ides in edible animal tissues[J].Food Chem,2014,(154):52-62.
[8]Peng D,Li Z,Wang Y,et al.Enzyme-linked immunoassay based on imprinted microspheres for the detection of sulfamethazine residue[J].JChromatogr A,2017,(1506):9-17.
[9]冯敏,李亚楠,高丼霞,等.酶联免疫吸附法在食品安全性指标检测中的研究迚展[J].食品安全质量检测学报,2016,7(10):3973-3979.Feng M,Li YN,Gao LX,et al.Research progress of enzyme-linked immunosorbent assay in food safety indices detection[J].J Food Saf Qual,2016,(10):3973-3979.
[10]田博,金坚,惠人杰,等.兽药残留检测中磺胺嘧啶ELISA试剂盒的研制[J].生物加工过程,2017,15(1):69-72.Tian B,Jin J,Hui RJ,et al.Determination of sulfadiazine in the veterinary drugs residue by sensitive ELISA[J].Chin J Bioprocess Eng,2017,15(1):69-72.
[11]苏明明,肖姗姗,张瑜,等.酶联免疫试剂盒检测牛血清中磺胺类药物残留[J].检验检疫学刊,2016,(2):17-19,30.Su MM,Xiao SS,Zhang Y,et al.The detection of sulfa drug residues using ELISA for bovine serum[J].J Inspect Quarant,2016,(2):17-19,30.
[12]李君华,米振杰,李志平,等.磺胺二甲嘧啶药物残留ELISA检测试剂盒的研制及初步应用[J].中国畜牧杂志,2013,(9):78-81.Li JH,Mi ZJ,Li ZP,et al.Development and preliminary application of ELISA kit for the detection of sulfamethazine residues[J]Chin J Anim Husband,2013,(9):78-81.
[13]罗贵昆,陈旭,谢体波,等.阿维菌素类药物酶联免疫快速检测试剂盒的制备及检测效果[J].中外食品工业,2014,(7):19-22.Luo GK,Chen X,Xie TB,et al.Preparation and effect of ELISA kit for rapid detection of abamectin[J].Global Food Ind,2014,(7):19-22.
[14]Ostermaier S,Schneider E,Usleber E,et al.Rapid enzyme immunoassays for the detection of three sulphonamides in milk[J].Food Agric Imunol,1995,7(3):253-258.
[15]张萍,陈燕,王晓玱.固相萃取-高效液相色谱法同时测定鸡蛋粉中12种磺胺类药物残留量药物[J].药物分析杂志,2010,30(12):2338-2343.Zhang P,Chen Y,Wang XL.Simultaneous determination of 12sulfonamide residues in egg powder by solid phase extraction and high performance liquid chromatography[J].J Pharm Anal,2010,30(12):2338-2343.
[16]陈吉之,闫超.饲料中9种磺胺类药物的HPLC法快速分离与检测[J].中国医药工业杂志,2015,6(8):892-894.Chen JZ,Yan C.Rapid separation and detection of 9 sulfonamides in feed by HPLC[J].Chin J Pharm Ind,2015,6(8):892-894.
[17]Zhang YP,Xu X,Qi X,et al.Determination of sulfonamides in livers using matix solid-phase dispersion extraction high-performance liquid chromatography[J].J Sparat Sci,2012,35(1):45-52.
[18]李雪德,鲜启明,刘红玱,等.高效液相色谱-荧光检测法同时测定蔬菜中3种磺胺类药物残留[J].分析化学,2010,38(3):429-433.Li XD,Xian QM,Liu HL,et al.Simultaneous determination of 3sulfonamides residues in vegetables by high performance liquid chromatography with fluorescence detection[J].Anal Chem,2010,38(3):429-433.
[19]吴翠琴,陈迪云,陈永亨,等.荧光胺衍生液相色谱法测定猪肝中10种磺胺[J].分析实验室,2018,37(12):1370-1374.Wu CQ,Chen DY,Chen YX,et al.Determination of 10 sulfonamides in pig liver by HPLC derived from fluorescein[J].Chin J Anal Lab,2018,37(12):1370-1374.
[20]王浩,启雷,殷晓燕,等.液相色谱-串联三重四极杆质谱对牛奶中10种磺胺类药物残留的同时测定[J].分析测试学报,2008,27(s):137-139.Wang H,Qi L,Yin XY,et al.Simultaneous determination of ten sulfonamides residues in mike by LC-MS/MS method[J].J Instrum Anal,2008,27(s):137-139.
[21]张晓强,张波,方萍,等.QuEChERS-超高效液相色谱-串联质谱法快速测定鱼肉中22种磺胺类药物残留[J].理化检验-化学分册,2015,51(3):369-374.Zhang XQ,Zhang B,Fang P,et al.Rapid determination of 22 sulfonamide residues in fish by QuEChERS-UPLC-MS/MS[J].Phys Test Chem Anal B,2015,51(3):369-374.
[22]Yu H,Tao YF,Chen DM,et al.Development of a high performance liquid chromatography method and a liquid chromatography-tandem mass spectrometry method with the pressurized liquid extraction for the quantification and confirmation of sulfonamides in the foods of animal origin[J].J Chromatogr B,2011,879(25):2653-2662.
[23]Heller DN,Ngoh MA,Donoghue D,et al.Identification of incurred sulfonamide residues in eggs:Methods for confirmation by liquid chromatography-tandem mass spectrometry and quantitation by liquid chromatography with ultraviolet detection[J].J Chromatogr B,2002,774(1):39-52.
[24]黄华,陈君慧,冯楠,等.动物源性食品中磺胺类药物残留前处理和检测方法研究迚展[J].食品工业科技,2013,34(4):378-381.Huang H,Chen JH,Feng N,et al.Research progress in the pre-processing and detection method of sulfonamides drugs residues in animal derived foods[J].Sci Technol Food Ind,2013,34(4):378-381.
[25]Pecorelli I,Bibi R,Fioroni L,et al.Validation of a confirmatory method for the determination of sulphonamides in muscle according to the European Union regulation 2002/657/EC[J].J Chromatogr A,2004,1032(1-2):23-29.
[26]Tso J,Agad S.A systematic investigation to optimize simultaneous extraction and liquid chromatography tandem mass spectrometry analysis of estrogens and their conjugated metabolites in milk[J].J Chromatogr A,2010,1217(29):4784-4795.
[27]Gomezperez ML,Romero-gonzalez R,Martinezvidal JL,et al.Analysis of veterinary drug residues in cheese by ultra-high-performance LC coupled to triple quadrupole MS/MS[J].J Sparat Si,2013,36(7):1223-1230.