分子印迹固相萃取LC-MS/MS法同时测定蜂蜜中11种氨基糖苷类抗生素
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摘要
目的建立蜂蜜中11种氨基糖苷类抗生素(链霉素、双氢链霉素、大观霉素、庆大霉素C1a、阿米卡星、西索米星、奈替米星、妥布霉素、潮霉素、巴龙霉素、卡那霉素)残留测定的分子印迹固相萃取-LC-MS/MS法。方法样品经50mmol/L磷酸二氢钾溶液提取,氨基糖苷类分子印迹固相萃取柱净化。以甲醇-0.3%甲酸-175mmol/L甲酸铵作为流动相,梯度洗脱,流速0.5 ml/min,柱温40℃。经ZIC-HILIC柱(50mm×2.1mm,3.5μm)分离,ESI~+-MS/MS检测,基质匹配标准曲线法定量。结果 11种待测物线性相关系数均大于0.997;检出限与定量限范围分别为0.002-0.025mg/kg和0.007-0.083 mg/kg;平均回收率范围为79.8%-95.0%;日内精密度与日间精密度分别低于15.4%与18.2%;11种待测物基质效应绝对值均小于16.2%。结论该方法选择性好、灵敏、准确、操作简便,可用于蜂蜜中11种氨基糖苷类抗生素的同时检测。
Objective To establish a method for simultaneous determination of 11 aminoglycoside antibiotics(AGs) including amikacin,puromycin,dihydrostreptomycin,gentamicin C1 a,hygromycin,kanamycin,netilmycin,spectinomycin,sisomicin,streptomycin and tobramycin in honey by LC-MS/MS with molecularly imprinted polymers solid phase extraction(MIPs SPE). Methods The aminoglycoside antibiotics in the honey sample were extracted with 50mmol/L potassium dihydrogen phosphate and then cleaned-up with MIPs SPE cartridges. The separation was performed on a ZIC-HILIC column(50 mm ×2. 1 mm,3. 5μm) with the mobile phase consisting of methanol,0. 3 % formic acid and 175mmol/L ammonium format at 0. 50ml/min in gradient elution. The MS/MS in positive ion mode was used for detection and the quantification was based on matrix-matched calibration curves. Results The linear correlation coefficients(r) of the target antibiotics were all greater than 0.997. The LODs of the method were 0. 002-0. 025 mg/kg and the LOQs were 0. 007-0. 083 mg/kg. The average recovery of this method ranged from 79. 8% to 95. 0%. The inter-day RSDs and intra-day RSDs were less than 15. 4% and 18. 2%,respectively and the absolute values of matrix effect for all AGs were less than 16. 2%. Conclusion The method is selective,sensitive,accurate,simple and suitable for simultaneous determination of 11 AGs residues in honey.
Objective To establish a method for simultaneous determination of 11 aminoglycoside antibiotics(AGs) including amikacin,puromycin,dihydrostreptomycin,gentamicin C1 a,hygromycin,kanamycin,netilmycin,spectinomycin,sisomicin,streptomycin and tobramycin in honey by LC-MS/MS with molecularly imprinted polymers solid phase extraction(MIPs SPE). Methods The aminoglycoside antibiotics in the honey sample were extracted with 50mmol/L potassium dihydrogen phosphate and then cleaned-up with MIPs SPE cartridges. The separation was performed on a ZIC-HILIC column(50 mm ×2. 1 mm,3. 5μm) with the mobile phase consisting of methanol,0. 3 % formic acid and 175mmol/L ammonium format at 0. 50ml/min in gradient elution. The MS/MS in positive ion mode was used for detection and the quantification was based on matrix-matched calibration curves. Results The linear correlation coefficients(r) of the target antibiotics were all greater than 0.997. The LODs of the method were 0. 002-0. 025 mg/kg and the LOQs were 0. 007-0. 083 mg/kg. The average recovery of this method ranged from 79. 8% to 95. 0%. The inter-day RSDs and intra-day RSDs were less than 15. 4% and 18. 2%,respectively and the absolute values of matrix effect for all AGs were less than 16. 2%. Conclusion The method is selective,sensitive,accurate,simple and suitable for simultaneous determination of 11 AGs residues in honey.
引文
[1]Kumar P,Rúbies A,CompanyóR,et al.Determination of aminoglycoside residues in kidney and honey samples by hydrophilic interaction chromatography-tandem mass spectrometry[J].Journal of Separation Science,2012,35(20):2710-2717.
[2]王志兵,高杨,刘洋,等.微波辅助衍生-离子液体分散液液微萃取-高效液相色谱法检测牛奶中氨基糖苷类抗生素残留[J].现代食品科技,2014,30(4):260-267.
[3]龚强,丁利,朱绍华,等.高效液相色谱-串联质谱法检测乳制品中10种氨基糖苷类抗生素残留[J].色谱,2012,30(11):1143-1147.
[4]Farouk F,Azzazy HM,Niessen WM.Challenges in the determination of aminoglycoside antibiotics,a review[J].Analytica Chimica Acta,2015,890:21-43.
[5]周茂金,梅如冰,苏美英.8种氨基糖苷类抗生素FDNB衍生化产物的电喷雾离子阱质谱及色谱行为研究[J].中国药学杂志,2011,46(6):458-462.
[6]莫文艳,黄燕华,曹俊明,等.柱前衍生化高效液相色谱法测定预混剂中硫酸安普霉素[J].药物分析杂志,2015,35(1):80-83.
[7]Chen SH,Liang YC,Chou YW.Analysis of kanamycin A in human plasma and in oral dosage form by derivatization with 1-naphthyl isothiocyanate and high-performance liquid chromatography[J].Journal of Separation Science,2006,29(5):607-612.
[8]Van Holthoon FL,Essers ML,Mulder PJ,et al.A generic method for the quantitative analysis of aminoglycosides(and spectinomycin)in animal tissue using methylated internal standards and liquid chromatography tandem mass spectrometry[J].Analytica Chimica Acta,2009,637(1/2):135-143.
[9]Kumar P,Rubies A,CompanyóR,et al.Hydrophilic interaction chromatography for the analysis of aminoglycosides[J].Journal of Separation Science,2012,35(4):498-504.
[10]Tao Y,Chen D,Yu H,et al.Simultaneous determination of 15aminoglycoside(s)residues in animal derived foods by automated solid-phase extraction and liquid chromatography-tandem mass spectrometry[J].Food Chemistry,2012,135(2):676-683.
[11]Breaud AR,Henemyre-Harris CL,Schools S,et al.Rapid quantification of the aminoglycoside arbekacin in serum using high performance liquid chromatography-tandem mass spectrometry[J].Clinica chimica acta;international journal of clinical chemistry,2013,418:102-106.
[12]Bohm DA,Stachel CS,Gowik P.Validation of a method for the determination of aminoglycosides in different matrices and species based on an in-house concept[J].Food additives&contaminants.Part A,Chemistry,analysis,control,exposure&risk assessment,2013,30(6):1037-1043.
[13]Kaufmann A,Butcher P,Maden K.Determination of aminoglycoside residues by liquid chromatography and tandem mass spectrometry in a variety of matrices[J].Analytica Chimica Acta,2012,711:46-53.
[14]Ishii R,Horie M,Chan W,et al.Multi-residue quantitation of aminoglycoside antibiotics in kidney and meat by liquid chromatography with tandem mass spectrometry[J].Food additives&contaminants.Part A,Chemistry,analysis,control,exposure&risk assessment,2008,25(12):1509-1519.
[15]Moreno-González D,Lara FJ,JurgovskáN,et al.Determination of aminoglycosides in honey by capillary electrophoresis tandem mass spectrometry and extraction with molecularly imprinted polymers[J].Analytica Chimica Acta,2015,891:321-328.
[2]王志兵,高杨,刘洋,等.微波辅助衍生-离子液体分散液液微萃取-高效液相色谱法检测牛奶中氨基糖苷类抗生素残留[J].现代食品科技,2014,30(4):260-267.
[3]龚强,丁利,朱绍华,等.高效液相色谱-串联质谱法检测乳制品中10种氨基糖苷类抗生素残留[J].色谱,2012,30(11):1143-1147.
[4]Farouk F,Azzazy HM,Niessen WM.Challenges in the determination of aminoglycoside antibiotics,a review[J].Analytica Chimica Acta,2015,890:21-43.
[5]周茂金,梅如冰,苏美英.8种氨基糖苷类抗生素FDNB衍生化产物的电喷雾离子阱质谱及色谱行为研究[J].中国药学杂志,2011,46(6):458-462.
[6]莫文艳,黄燕华,曹俊明,等.柱前衍生化高效液相色谱法测定预混剂中硫酸安普霉素[J].药物分析杂志,2015,35(1):80-83.
[7]Chen SH,Liang YC,Chou YW.Analysis of kanamycin A in human plasma and in oral dosage form by derivatization with 1-naphthyl isothiocyanate and high-performance liquid chromatography[J].Journal of Separation Science,2006,29(5):607-612.
[8]Van Holthoon FL,Essers ML,Mulder PJ,et al.A generic method for the quantitative analysis of aminoglycosides(and spectinomycin)in animal tissue using methylated internal standards and liquid chromatography tandem mass spectrometry[J].Analytica Chimica Acta,2009,637(1/2):135-143.
[9]Kumar P,Rubies A,CompanyóR,et al.Hydrophilic interaction chromatography for the analysis of aminoglycosides[J].Journal of Separation Science,2012,35(4):498-504.
[10]Tao Y,Chen D,Yu H,et al.Simultaneous determination of 15aminoglycoside(s)residues in animal derived foods by automated solid-phase extraction and liquid chromatography-tandem mass spectrometry[J].Food Chemistry,2012,135(2):676-683.
[11]Breaud AR,Henemyre-Harris CL,Schools S,et al.Rapid quantification of the aminoglycoside arbekacin in serum using high performance liquid chromatography-tandem mass spectrometry[J].Clinica chimica acta;international journal of clinical chemistry,2013,418:102-106.
[12]Bohm DA,Stachel CS,Gowik P.Validation of a method for the determination of aminoglycosides in different matrices and species based on an in-house concept[J].Food additives&contaminants.Part A,Chemistry,analysis,control,exposure&risk assessment,2013,30(6):1037-1043.
[13]Kaufmann A,Butcher P,Maden K.Determination of aminoglycoside residues by liquid chromatography and tandem mass spectrometry in a variety of matrices[J].Analytica Chimica Acta,2012,711:46-53.
[14]Ishii R,Horie M,Chan W,et al.Multi-residue quantitation of aminoglycoside antibiotics in kidney and meat by liquid chromatography with tandem mass spectrometry[J].Food additives&contaminants.Part A,Chemistry,analysis,control,exposure&risk assessment,2008,25(12):1509-1519.
[15]Moreno-González D,Lara FJ,JurgovskáN,et al.Determination of aminoglycosides in honey by capillary electrophoresis tandem mass spectrometry and extraction with molecularly imprinted polymers[J].Analytica Chimica Acta,2015,891:321-328.