液相色谱-串联质谱法测定水产品中亮绿、亚甲基蓝及其代谢物残留量
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摘要
建立了水产品中亮绿、亚甲基蓝及其代谢物残留量同时测定的液相色谱-串联质谱(LC-MS/MS)方法。样品经乙酸铵缓冲溶液和乙腈提取,二氯甲烷液液萃取,PRS固相萃取柱净化,氮吹浓缩,定容后测定。以2 mmol/L乙酸铵(含0. 1%甲酸)、乙腈和甲醇为流动相,CAPCELL PAK C_(18)色谱柱进行分离,在选择反应监测(SRM)模式下测定,外标法定量。在最佳实验条件下,5种化合物在1. 0～100. 0μg/L范围内线性关系良好(r~2> 0. 999),检出限(LOD,S/N≥3)均为1. 0μg/kg,定量下限(LOQ,S/N≥10)均为2. 0μg/kg;在水产品中加标水平为1. 0、5. 0、10. 0μg/kg时,回收率为70. 3%～92. 1%,相对标准偏差(RSD,n=6)为2. 3%～13%。该方法灵敏度高,能有效检测水产品中亮绿、亚甲基蓝及其代谢物的残留量。
A liquid chromatography-tandem mass spectrometric( LC-MS/MS) method was developed for the determination of brilliant green,methylene blue and their metabolites in aquatic products. The samples were extracted with ammonium acetate buffer solution and acetonitrile,followed by extraction with dichloromethane,then purified on a PRS solid phase extraction column. The eluent was concentrated by nitrogen blowing,diluted to a certain volume and determined. The targets were separated on a CAPCELL PAK C_(18) column with 2 mmol/L aqueous ammonium acetate containing 0. 1% formic acid,acetonitrile and methanol as mobile phases. The determination of the analytes was performed by LC-MS/MS in selected reaction monitoring( SRM) mode,and the external standard method was used for quantitation. There existed good linear relationships for the analytes in the range of 1. 0-100. 0 μg/L with their correlation coefficients( r~2) larger than 0. 999. The limits of detection( LOD,S/N≥3) and quantitation( LOQ,S/N≥10) were 1. 0 μg/kg and 2. 0 μg/kg,respectively. The average recoveries at three spiked levels of 1. 0,5. 0 and 10. 0 μg/kg were in the range of 70. 3%-92. 1% with their relative standard deviations( RSDs,n = 6) of 2. 3%-13%.The method has high sensitivity and could be used in the effective detection on residues of brilliant green,methylene blue and their metabolites in aquatic products.
A liquid chromatography-tandem mass spectrometric( LC-MS/MS) method was developed for the determination of brilliant green,methylene blue and their metabolites in aquatic products. The samples were extracted with ammonium acetate buffer solution and acetonitrile,followed by extraction with dichloromethane,then purified on a PRS solid phase extraction column. The eluent was concentrated by nitrogen blowing,diluted to a certain volume and determined. The targets were separated on a CAPCELL PAK C_(18) column with 2 mmol/L aqueous ammonium acetate containing 0. 1% formic acid,acetonitrile and methanol as mobile phases. The determination of the analytes was performed by LC-MS/MS in selected reaction monitoring( SRM) mode,and the external standard method was used for quantitation. There existed good linear relationships for the analytes in the range of 1. 0-100. 0 μg/L with their correlation coefficients( r~2) larger than 0. 999. The limits of detection( LOD,S/N≥3) and quantitation( LOQ,S/N≥10) were 1. 0 μg/kg and 2. 0 μg/kg,respectively. The average recoveries at three spiked levels of 1. 0,5. 0 and 10. 0 μg/kg were in the range of 70. 3%-92. 1% with their relative standard deviations( RSDs,n = 6) of 2. 3%-13%.The method has high sensitivity and could be used in the effective detection on residues of brilliant green,methylene blue and their metabolites in aquatic products.
引文
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[2]Zhai Y X,Guo Y Y,Geng X,Zhang C,Ning J S.Periodical of Ocean University of China(翟毓秀,郭莹莹,耿霞,张翠,宁劲松.中国海洋大学学报),2007,37(1):27-32.
[3]Lopez-Gutierrez N,Romero-Gonzalez R,Vidal J L M,Frenich A G.Anal.Methods,2013,5:3434-3449.
[4]Tavallali H,Ostovar M.Int.J.Chem.Technol.Res.,2009,1:199-203.
[5]Yang F,Liu Z C,Hu X Z,Lin Y F,Chen G N.J.Pharm.Anal.(杨方,刘正才,胡小钟,林雁飞,陈国南.药物分析杂志),2008,28(8):1395-1400.
[6]Chen W G,Qu J P,Zhou F N.Guangdong Agric.Sci.(陈万光,屈菊平,周芬娜.广东农业科学),2010,37(5):131-132.
[7]Di Santo A R,Wagner J G.J.Pharm.Sci.,1972,61(4):598-602.
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[9]Borwitzky H,Haefeli W E,Burhenne J.J.Chromatogr.B,2005,826(1):244-251.
[10]Yang F,Xia S F,Liu Z C,Chen J,Lin Y H,Qiu B,Chen G N.Electrophoresis,2011,32(6/7):659-664.
[11]Cai S T.Fujian Anal.Test.(蔡素婷.福建分析测试),2015,24(1):6-10.
[12]Gu L,Yan J,Ke M,Liu Y P,Shi A H.Chin.J.Anal.Lab.(顾玲,闫璟,柯苗,刘彦平,石爱华.分析试验室),2016,35(8):966-970.
[13]Wang Y,Yu H J,Qian B L,Huang D M,Hui Y H,Cai Y Q.Chin.J.Anal.Lab.(王媛,于慧娟,钱蓓蕾,黄冬梅,惠芸华,蔡友琼.分析试验室),2013,32(1):90-94.
[14]Long J,Li Z M,Yu L,Li P P,Yan Z Y,Zhang X J.Anhui Agric.Sci.(龙举,李子孟,喻亮,李佩佩,严忠雍,张小军.安徽农业科学),2015,43(24):5-6.
[15]Hou J B,Xie W,Zhu Z L,Zeng G N,LüC H,He J M.Phys.Test.Chem.Anal.:Chem.Anal.(侯建波,谢文,祝泽龙,曾淦宁,吕春华,何建敏.理化检验-化学分册),2015,51(3):403-408.
[16]Amelin V G,Korotkov A I,Andoralov A M.J.Anal.Chem.,2017,72(2):183-190.
[17]Hurtaud-Pessel D,Cou3dor P,Verdon E.J.Chromatogr.A,2011,1218(12):1632-1645.
[18]Li B R.Application of the HPLC-MS/MS Method in Food Safety Analysis.Changsha:Hunan University(李帮锐.高效液相色谱-串联质谱联用法在食品安全分析中的应用.长沙:湖南大学),2010.
[19]Hui Y H,Zhang X,Huang D M,Wang Y,Yu H J.J.Anal.Sci.(惠芸华,张璇,黄冬梅,王媛,于慧娟.分析科学学报),2015,31(4):533-536.
[20]Tarbin J A,Chan D,Stubbings G,Sharman M.Anal.Chim.Acta,2008,625(2):188-194.
[21]Zhou Y,Zhao Y G,Zhang B B,Zhang Y,Chen G S.Chin.J.Anal.Chem.(周岩,赵永刚,张蓓蓓,章勇,陈国松.分析化学),2014,42(3):367-374.
[22]Wu Y B,Wang J H,Li G L.Hunan Agric.Sci.(吴艳兵,王建华,李广领.湖南农业科学),2008,(3):165-167.
[23]Zhang Y,Feng C X,Chen J G,Liang S D.Chin.J.Health Lab.Technol.(张艳,冯翠霞,陈剑刚,梁素丹.中国卫生检验杂志),2017,27(10):1385-1388.
[24]Li X L,Li N,Li P,Liu L,Miao H.Chin.J.Food Hyg.(李晓丽,李娜,李鹏,刘力,苗虹.中国食品卫生杂志),2012,24(3):209-214.
[25]Yang F,Fan K W,Liu Z C,Wu D F,Lin Y H,Chen J,Chen G N.J.Instrum.Anal.(杨方,范克伟,刘正才,吴德峰,林永辉,陈健,陈国南.分析测试学报),2009,28(1):32-36.
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[27]Yao M K,Ma B L,Ma Y M.J.Pharm.Anal.(姚梦侃,马秉亮,马越鸣.药物分析杂志),2010,30(12):2436-2440.
[28]Zhu L,Wang C,Chen H P,Zhang Y B,Zhou S J,Wang G Q,Liu X.Chin.J.Anal.Chem.(诸力,王晨,陈红平,张颖彬,周苏娟,王国庆,刘新.分析化学),2017,45(4):529-536.
[29]Cui J,Yang H S,Zhang J H,Wu G H.J.Fish.Sci.South China(崔瑾,杨洪生,章建浩,吴光红.南方水产科学),2013,9(3):67-73.