冷鲜肉中β-受体激动剂测定方法的比对及优化研究
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摘要
目的对盐酸克伦特罗、莱克多巴胺、沙丁胺醇的现有检测方法进行比对,并经优化得到一种基于超高效液相色谱-串联质谱(ultra high performance liquid chromatography-tandem mass spectrometry,UPLC-MS/MS)的检测方法。方法对2种现行检测标准和QuEChERS方法进行方法确认比对,并基于标准方法原理进行逐步优化。通过酶解、无机提取、调pH、有机提取、固相萃取、浓缩过程进行前处理,并通过UPLC-MS/MS对冷鲜肉中盐酸克伦特罗、莱克多巴胺和沙丁胺醇进行分析。结果该优化方法定量限在0.08～0.17μg/kg区间,3个浓度的加标回收率在81.4%～94.6%区间,相对标准偏差(relative standard deviation,RSD)小于8.1%(n=5).结论该方法相比标准方法,前处理时间缩短一半以上,仪器分析效率也有所提高;相比于QuEChERS方法具有更低的定量限和更稳定的回收率。
Objective To compare the available methods for determination of clenbuterol hydrochloride,ractopamine and salbutamol, and obtain an optimized detection method based on high performance liquid chromatography tandem mass spectrometry(UPLC-MS/MS). Methods Two kinds of available standard methods and QuEChERS methods were employed for validation and comparison, following optimization step by step based on the principle of standard method. Clenbuterol hydrochloride, lake dopamine and salbutamol in chilled meat were analyzed by pretreatment including enzyme hydrolysis, inorganic extraction, pH adjustment, organic extraction, solid phase extraction, concentration, and detected by UPLC-MS/MS. Results The limit of quantitation of method were0.08-0.17 μg/kg. The recoveries at 3 spiked levels were 81.4%-94.6%, and the relative standard deviations(RSDs)were less than 8.1%(n=5). Conclusion Compared with the standard method, the pretreatment time of this method is more than half, and the efficiency of instrumental analysis is improved. Compared with QuEChERS method, it has lower limit of quantitation and more stable recovery rate.
Objective To compare the available methods for determination of clenbuterol hydrochloride,ractopamine and salbutamol, and obtain an optimized detection method based on high performance liquid chromatography tandem mass spectrometry(UPLC-MS/MS). Methods Two kinds of available standard methods and QuEChERS methods were employed for validation and comparison, following optimization step by step based on the principle of standard method. Clenbuterol hydrochloride, lake dopamine and salbutamol in chilled meat were analyzed by pretreatment including enzyme hydrolysis, inorganic extraction, pH adjustment, organic extraction, solid phase extraction, concentration, and detected by UPLC-MS/MS. Results The limit of quantitation of method were0.08-0.17 μg/kg. The recoveries at 3 spiked levels were 81.4%-94.6%, and the relative standard deviations(RSDs)were less than 8.1%(n=5). Conclusion Compared with the standard method, the pretreatment time of this method is more than half, and the efficiency of instrumental analysis is improved. Compared with QuEChERS method, it has lower limit of quantitation and more stable recovery rate.
引文
[1]孙雷,张骊,朱永林,等.超高效液相色谱-串联质谱法检测动物源性食品中残留的9种β-受体激动剂[J].色谱,2018, 26(6):709-713.Sun L, Zhang L, Zhu YL, et al. Simulaneous determination of nineβ-agonist residues in animal derived foods by ultra performance liquid chromatography-tandem mass spectrometry[J]. Chin J Chromatogr, 2018,26(6):709-713.
[2]张清安,范学辉.动物性食品中盐酸克伦特罗(瘦肉精)残留危害及其检测方法研究进展[J].食品与发酵工业,2004,30(9):108-111,119.Zhang QA, Fan XH. Hazard of clenbuterol residual in animal food and research progress on its determination method[J]. Food Ferment Ind, 2004,30(9):108-111,119.
[3] GB/T22286-2008动物源性食品中多种β-受体激动剂残留量的测定液相色谱串联质谱法[S].GB/T 22286-2008 Determination ofβ-agonists residues in foodstuff of animal origin-Liquid chromatography with tandem-mass spectrometric method[S].
[4]农业部1025号公告-18-2008动物源性食品中β-受体激动剂残留检测液相色谱-串联质谱法[S].Announcement No. 1025 of the Ministry of agriculture-18-2008Determination ofβ-agonists residues in animal derived food by liquid chromatography-tandem mass spectrometry[S].
[5]高洁,苗虹.兽药残留检测技术研究进展[J].食品安全质量检测学报,2013,4(1):14-16.Gao J, Miao H. Recent development of analytical methods for veterinary drug residues[J]. J Food Saf Qual, 2013,4(1):14-16.
[6]汤轶伟,王硕,励建荣,等.β-兴奋剂盐酸克伦特罗残留检测方法最新研究进展[J].中国食品学报,2013,5(13):155-160.Tang YW, Wang S, Li JR, et al. Recent developments of detecting clenbuterol hydrochloride residues in different samples[J]. J Food Sci Technol, 2013,5(13):154-160.
[7] Simon T, Shellaiah M, Steffi P, et al. Development of extremely stable dual functionalized gold nanoparticles for effective colorimetric detection of clenbuterol and ractopamine in human urine samples[J]. Anal Chim Acta, 2018, 1023:96-104.
[8] Lehotay S, MastovskáK, Yun S. Evaluation of two fast and easy methods for pesticide residue analysis in fatty food matrixes[J]. AOAC Int, 2005,88(2):630-638.
[9] González-Curbelo M, Socas-Rodriguez B, Herrera-Herrera A, et al.Evolution and applications of the QuEChERS method[J]. TrAC Trends Anal Chem, 2015, 71:169-185.
[10] Qin Y, Zhang J, Li Y, et al. Automated multi-filtration cleanup with nitrogen-enriched activated carbon material as pesticide multi-residue analysis method in representative crop commodities[J]. J Chromatogr A,2017, 1515:62-68.
[11]许秀敏,龙朝阳,黄伟雄,等.QuEChERS-超高效液相色谱-串联质谱法同时快速检测果蔬中35种甲氧基丙烯酸酯类和三唑类杀菌剂的残留量[J].食品安全质量检测学报,2019,10(4):1039-1047.Xu XM, Long CY, Huang WX, et al. Simultaneous rapid determination of35 methoxyacrylate and triazole fungicides in fruits and vegetables by QuEChERS-ultra-high performance liquid chromatography-tandem mass spectrometry[J]. J Food Saf Qual, 2019,10(4):1039-1047.
[12]金婷,孙欣,李卓瓦,等.QuEChERS-气相色谱-三重四极杆质谱法检测石榴中的19种含磷农药残留[J/OL].食品与发酵工业.https://doi.org/10.13995/j.cnki. 11-1802/ts.015976Jin T,Sun X,Li ZW,et al. Determination of 19 pesticide residues in pomegranates using QuEChERS coupled with gas chromatography-triple quadrupole mass spectrometry[J/OL]. Food Ferment Ind,https://doi.org/10.13995/j.cnki. 11-1802/ts.015976
[13] González-Jartin JM, Alfonso A, Rodriguez I, et al. A QuEChERS based extraction procedure coupled to UPLC-MS/MS detection for mycotoxins analysis in beer[J]. Food Chem, 2019, 275:703-710.
[14] Santos AG, Regis ACD, Da-Rocha GO, et al. A simple, comprehensive,and miniaturized solvent extraction method for determination of particulate-phase polycyclic aromatic compounds in air[J]. J Chromatogr A, 2016,1435:6-17.
[15]李帅,陈辉,金铃和,等.高效液相色谱-串联质谱法测定蜂蜜中20种全氟烷基化合物[J].色谱,2017, 5(35):495-501.Li S, Chen H, Jin LH, et al. Determination of 20 perfluorted alkyl substances in honey by high performance liquid chromatography-tandem mass spectrometry[J]. Chin J Chromatogr, 2017, 5(35):495-501.
[16]陈磊,吴赟琦,赵志勇,等.QuEChERS/超高效液相色谱-串联质谱法快速测定土壤中19种氟喹诺酮类抗生素残留[J].分析测试学报,2019,2(38):194-200.Chen L, Wu YQ, Zhao ZY, et al. Rapid determination of 19fluoroquinolones antibiotic residues in soil by quechers/ultra performance liquid chromatography-tandem mass spectrometry[J]. J Instrum Anal,2019,2(38):194-200.
[17] Dclatour T, Racault L, Bessaire T, et al. Screening of veterinary drug residues in food by LC-MS/MS. Background and challenges[J]. Food Addit Contam A, 2018, 35(4):632-645.
[18]曲斌.耿士伟,陆桂萍,等.新型QuEChERS方法结合液相色谱串联质谱法快速测定猪肝中β-受体激动剂残留[J].食品安全质量检测学报,2015, 12(6):4748-4754.Qu B, Geng SW, Lu GP, et al. Rapid determination ofβ-agonists residuals in pig liver by liquid chromatography-tandem mass spectrometry combined with novel QuEChERS method[J]. J Food Saf Qual, 2015,12(6):4748-4754.
[19]郭海霞,肖桂英,张禧庆,等.QuEChERS-超高效液相色谱-串联质谱法同时检测猪肉中121种兽药[J].色谱,2015, 33(12):1242-1250.Guo HX, Xiao GY, Zhang XQ, et al. Simultaneous determination of 121veterinary drugs in pork by QuEChERS and ultra performance liquid chromatography-tandem mass spectrometry[J]. Chin J Chromatogr, 2015,33(12):1242-1250.
[2]张清安,范学辉.动物性食品中盐酸克伦特罗(瘦肉精)残留危害及其检测方法研究进展[J].食品与发酵工业,2004,30(9):108-111,119.Zhang QA, Fan XH. Hazard of clenbuterol residual in animal food and research progress on its determination method[J]. Food Ferment Ind, 2004,30(9):108-111,119.
[3] GB/T22286-2008动物源性食品中多种β-受体激动剂残留量的测定液相色谱串联质谱法[S].GB/T 22286-2008 Determination ofβ-agonists residues in foodstuff of animal origin-Liquid chromatography with tandem-mass spectrometric method[S].
[4]农业部1025号公告-18-2008动物源性食品中β-受体激动剂残留检测液相色谱-串联质谱法[S].Announcement No. 1025 of the Ministry of agriculture-18-2008Determination ofβ-agonists residues in animal derived food by liquid chromatography-tandem mass spectrometry[S].
[5]高洁,苗虹.兽药残留检测技术研究进展[J].食品安全质量检测学报,2013,4(1):14-16.Gao J, Miao H. Recent development of analytical methods for veterinary drug residues[J]. J Food Saf Qual, 2013,4(1):14-16.
[6]汤轶伟,王硕,励建荣,等.β-兴奋剂盐酸克伦特罗残留检测方法最新研究进展[J].中国食品学报,2013,5(13):155-160.Tang YW, Wang S, Li JR, et al. Recent developments of detecting clenbuterol hydrochloride residues in different samples[J]. J Food Sci Technol, 2013,5(13):154-160.
[7] Simon T, Shellaiah M, Steffi P, et al. Development of extremely stable dual functionalized gold nanoparticles for effective colorimetric detection of clenbuterol and ractopamine in human urine samples[J]. Anal Chim Acta, 2018, 1023:96-104.
[8] Lehotay S, MastovskáK, Yun S. Evaluation of two fast and easy methods for pesticide residue analysis in fatty food matrixes[J]. AOAC Int, 2005,88(2):630-638.
[9] González-Curbelo M, Socas-Rodriguez B, Herrera-Herrera A, et al.Evolution and applications of the QuEChERS method[J]. TrAC Trends Anal Chem, 2015, 71:169-185.
[10] Qin Y, Zhang J, Li Y, et al. Automated multi-filtration cleanup with nitrogen-enriched activated carbon material as pesticide multi-residue analysis method in representative crop commodities[J]. J Chromatogr A,2017, 1515:62-68.
[11]许秀敏,龙朝阳,黄伟雄,等.QuEChERS-超高效液相色谱-串联质谱法同时快速检测果蔬中35种甲氧基丙烯酸酯类和三唑类杀菌剂的残留量[J].食品安全质量检测学报,2019,10(4):1039-1047.Xu XM, Long CY, Huang WX, et al. Simultaneous rapid determination of35 methoxyacrylate and triazole fungicides in fruits and vegetables by QuEChERS-ultra-high performance liquid chromatography-tandem mass spectrometry[J]. J Food Saf Qual, 2019,10(4):1039-1047.
[12]金婷,孙欣,李卓瓦,等.QuEChERS-气相色谱-三重四极杆质谱法检测石榴中的19种含磷农药残留[J/OL].食品与发酵工业.https://doi.org/10.13995/j.cnki. 11-1802/ts.015976Jin T,Sun X,Li ZW,et al. Determination of 19 pesticide residues in pomegranates using QuEChERS coupled with gas chromatography-triple quadrupole mass spectrometry[J/OL]. Food Ferment Ind,https://doi.org/10.13995/j.cnki. 11-1802/ts.015976
[13] González-Jartin JM, Alfonso A, Rodriguez I, et al. A QuEChERS based extraction procedure coupled to UPLC-MS/MS detection for mycotoxins analysis in beer[J]. Food Chem, 2019, 275:703-710.
[14] Santos AG, Regis ACD, Da-Rocha GO, et al. A simple, comprehensive,and miniaturized solvent extraction method for determination of particulate-phase polycyclic aromatic compounds in air[J]. J Chromatogr A, 2016,1435:6-17.
[15]李帅,陈辉,金铃和,等.高效液相色谱-串联质谱法测定蜂蜜中20种全氟烷基化合物[J].色谱,2017, 5(35):495-501.Li S, Chen H, Jin LH, et al. Determination of 20 perfluorted alkyl substances in honey by high performance liquid chromatography-tandem mass spectrometry[J]. Chin J Chromatogr, 2017, 5(35):495-501.
[16]陈磊,吴赟琦,赵志勇,等.QuEChERS/超高效液相色谱-串联质谱法快速测定土壤中19种氟喹诺酮类抗生素残留[J].分析测试学报,2019,2(38):194-200.Chen L, Wu YQ, Zhao ZY, et al. Rapid determination of 19fluoroquinolones antibiotic residues in soil by quechers/ultra performance liquid chromatography-tandem mass spectrometry[J]. J Instrum Anal,2019,2(38):194-200.
[17] Dclatour T, Racault L, Bessaire T, et al. Screening of veterinary drug residues in food by LC-MS/MS. Background and challenges[J]. Food Addit Contam A, 2018, 35(4):632-645.
[18]曲斌.耿士伟,陆桂萍,等.新型QuEChERS方法结合液相色谱串联质谱法快速测定猪肝中β-受体激动剂残留[J].食品安全质量检测学报,2015, 12(6):4748-4754.Qu B, Geng SW, Lu GP, et al. Rapid determination ofβ-agonists residuals in pig liver by liquid chromatography-tandem mass spectrometry combined with novel QuEChERS method[J]. J Food Saf Qual, 2015,12(6):4748-4754.
[19]郭海霞,肖桂英,张禧庆,等.QuEChERS-超高效液相色谱-串联质谱法同时检测猪肉中121种兽药[J].色谱,2015, 33(12):1242-1250.Guo HX, Xiao GY, Zhang XQ, et al. Simultaneous determination of 121veterinary drugs in pork by QuEChERS and ultra performance liquid chromatography-tandem mass spectrometry[J]. Chin J Chromatogr, 2015,33(12):1242-1250.