超高效液相色谱-串联质谱法检测茶制品中非法添加13种抗风湿类药物
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摘要
目的建立超高效液相色谱-串联质谱法检测茶制品中非法添加13种抗风湿类药物(氨基比林、对乙酰氨基酚、甲氧苄啶、氢化可的松、吡罗昔康、醋酸泼尼松、地塞米松、双氯芬酸钠、吲哚美辛、保泰松、罗通定、安替比林、非那西丁)的分析方法。方法样品甲醇超声提取后,以0.1%的甲酸溶液-乙腈为流动相梯度洗脱,经Inertsil ODS-3(2.1 mm×75 mm, 2μm)色谱柱分离,目标化合物在ESI源正离子模式下电离,采用多反应监测模式进行定性、定量分析。结果 13种抗风湿的方法检出限(S/N=3)为0.3～1.6μg/kg,定量限(S/N=10)为1.4～6.5μg/kg。在低、中、高3个加标水平下的平均回收率为80.20%～110.31%。对25批次市售抗风湿类茶制品进行检测,均未发现上述13种抗风湿类药物。结论该方法灵敏高、专属性强,适用于茶制品中抗风湿类非法添加的定量及确证分析。
Objective To establish a method for rapid determination of 13 kinds of anti-rheumatic drugs(aminophenazone, 4-acetamidophenol, trimethoprim, hydrocortisone, piroxicam, prednisone 21-acetate,dexamethasone, phenacetin, indometacin, phenylbutazone, rotundine, phenazone, diclofenac sodium) added in tea products by ultra performance liquid chromatography-tandem mass spectrometry. Methods The samples were extracted with methanol by ultrasonication. After chromatographic separation on an Inertsil ODS-3(2.1 mm×75 mm,2 μm) column with 0.1% formic acid solution-acetonitrile as mobile phase, the target compounds were qualitatively and quantitatively determined under the multiple reaction monitoring(MRM) mode in positive ionization mode.Results The limits of detection(LOD) for 13 anti-rheumatic were in the range of 0.3-1.6 μg/kg and the limits of quantification(LOQ) were in the range of 1.4-6.5 μg/kg. The average recoveries at three spiked levels ranged from80.20% to 110.31%. None of the 13 anti-rheumatic drugs were found in 25 batches of commercially available anti-rheumatic tea products. Conclusion This method is sensitive, sufficiently selective and is suitable for the determination and confirmation of 13 anti-rheumatic in tea products.
Objective To establish a method for rapid determination of 13 kinds of anti-rheumatic drugs(aminophenazone, 4-acetamidophenol, trimethoprim, hydrocortisone, piroxicam, prednisone 21-acetate,dexamethasone, phenacetin, indometacin, phenylbutazone, rotundine, phenazone, diclofenac sodium) added in tea products by ultra performance liquid chromatography-tandem mass spectrometry. Methods The samples were extracted with methanol by ultrasonication. After chromatographic separation on an Inertsil ODS-3(2.1 mm×75 mm,2 μm) column with 0.1% formic acid solution-acetonitrile as mobile phase, the target compounds were qualitatively and quantitatively determined under the multiple reaction monitoring(MRM) mode in positive ionization mode.Results The limits of detection(LOD) for 13 anti-rheumatic were in the range of 0.3-1.6 μg/kg and the limits of quantification(LOQ) were in the range of 1.4-6.5 μg/kg. The average recoveries at three spiked levels ranged from80.20% to 110.31%. None of the 13 anti-rheumatic drugs were found in 25 batches of commercially available anti-rheumatic tea products. Conclusion This method is sensitive, sufficiently selective and is suitable for the determination and confirmation of 13 anti-rheumatic in tea products.
引文
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[13]肖延民.糖皮质激素类药物的临床应用研究[J].北方药学2019,16(3):172-173.Xiao YM.Clinical application of glucocorticoids[J].Northern Pharm,2019,16(3):172-173.
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[17]翁昆,方晨,张亚丽.茶叶标准体系研究[J].中国茶叶加工,2011,(4):14-17.Weng K,Fang C,Zhang YL.Study on tea standard system[J].China Tea Process,2011,(4):14-17.
[18]翁昆,黄皓.论我国茶叶标准体系的建设[J].中国茶叶加工,2009,(3):3-6.Weng K,Huang H.On establishing standard system for tea in China[J].China Tea Process,2009,(3):3-6.
[19]周建良,方翠芬.快速液相色谱-串联质谱联用同时检测抗风湿类中药制剂中13种添加化学药物成分[J].药物分析杂志,2013,33(2):281-285.Zhou JL,Fang CF.Rapid liquid chromatography-tandem mass spectrometry for simultaneous determination of 13 additive chemical components in anti-rheumatic traditional Chinese medicine preparations[J].J Pharm Anal,2013,33(2):281-285.
[20]黎雪清,谭渺.HPLC法快速筛查抗风湿类中成药和保健食品中24种非法添加化学成分[J].中成药,2014,36(9):1891-1894.Li XQ,Tan M.Rapid screening of 24 illegally added chemical constituents in anti-rheumatic Chinese patent medicines and health food by high performance liquid chromatography[J].Chin Patent Med,2014,36(9):1891-1894.
[21]廖瑜.HPLC快速筛查抗风湿类中成药及保健品中非法添加的10种化学药[J].中国现代应用药学,2014,31(7):868-871.Liao Y.Rapid screening of 10 chemicals illegally added in Chinese patent anti-rheumatic drugs and health products by high performance liquid chromatography[J].Mod Appl Pharm China,2014,31(7):868-871.
[2]李莉,安冬青,李凯利,等.山明茶对高尿酸血症患者代谢指标及血栓前标志物的影响[J].湖南中医杂志,2012,28(3):22-24,28.Li L,An DQ,Li KL,et al.The effects of Shanming tea on metabolic indices and pre-thrombotic markers in patients with hyperuricemia[J].Hunan J Tradit Chin Med,2012,28(3):22-24,28.
[3]黎雪清,谭渺,蒋创杰,等.HPLC法快速筛查抗风湿类中成药和保健食品中24种非法添加化学成分[J].中成药,2014,36(9):1891-1894.Li XQ,Tan M,Jiang CJ,et al.Rapid screening of 24 illegally added chemical components in anti-rheumatic Chinese patent medicines and health food by HPLC[J].Chin Patent Med,2014,36(9):1891-1894.
[4]李强,岳磊,李晓静.UPLC-MS/MS法快速筛查抗风湿类中药贴剂中非法添加的17种化学药物成分[J].中国药房,2017,28(12):1692-1696.Li Q,Yue L,Li XJ.UPLC-MS/MS method for rapid screening of 17chemicals illegally added in anti-rheumatic traditional Chinese medicine patches[J].China Pharm,2017,28(12):1692-1696.
[5]国家药典委员会.中华人民共和国药典2部[M].北京:中国医药科技出版社,2015.State Pharmacopoeia Commission.Two pharmacopoeia departments of the People's Republic of China[M].Beijing:China Pharmaceutical Science and Technology Publishing House,2015.
[6]陈梓云,姚婉清,彭梦侠.红外光谱结合判别分析法快速筛查抗风湿类中成药中的氨基比林[J].化学研究与应用,2018,(10):1703-1707.Chen ZY,Yao WQ,Peng MX.Rapid screening of aminopyrine in anti-rheumatic Chinese patent medicines by infrared spectroscopy combined with discriminant analysis[J].Chem Res Appl,2018,(10):1703-1707.
[7]徐军辉,李存金,王仕平,等.中成药中非法添加吲哚美辛检测方法的研究[J].中国药事,2010,24(9):894.Xu JH,Li CJ,Wang SP,et al.Study on the determination method of indomethacin illegally added in Chinese patent medicines[J].Chin Pharm Matters,2010,24(9):894.
[8]陈梓云,姚婉清,彭梦侠.红外光谱结合判别分析法快速筛查抗风湿类中成药中的吡罗昔康[J].化学世界,2018,59(11):722-727.Chen ZY,Yao WQ,Peng MX.Rapid screening of piroxicam in anti-rheumatic Chinese patent medicines by infrared spectroscopy combined with discriminant analysis[J].Chem World,2018,59(11):722-727.
[9]年永琼,辛元尧,杨建鑫,等.模拟低氧环境对对乙酰氨基酚药代动力学的影响[J].华西药学杂志,2019,34(2):141-146.Nian YQ,Xin YY,Yang JX,et al.Effects of simulated hypoxia on the pharmacokinetics of paracetamol[J].Western China J Pharm,2019,34(2):141-146.
[10]柳亚玲,陈泳,李正全,等.吲哚美辛的波谱学数据与结构确证[J].广东化工,2018,45(19):44-46.Liu YL,Chen Y,Li ZQ,et al.Spectroscopic data and structural confirmation of indomethacin[J].Guangdong Chem Ind,2018,45(19):44-46.
[11]何睿偲,黄艳婷,雷毅,等.HPLC法快速筛查抗风湿类中成药或保健食品中21种非法添加化学成分[J].分析测试学报,2016,35(11):1486-1490.He RX,Huang YT,Lei Y,et al.Rapid screening of 21 illegally added chemical constituents in anti-rheumatic Chinese patent medicines or health foods by HPLC[J].J Instrum Anal,2016,35(11):1486-1490.
[12]刘清妹.氢化可的松治疗肺炎支原体引起的小儿大叶性肺炎51例疗效观察[J].当代医学,2019,25(6):95-97.Liu QM.Therapeutic effect of hydrocortisone on 51 children with lobar pneumonia caused by Mycoplasma pneumoniae[J].Contemp Med,2019,25(6):95-97.
[13]肖延民.糖皮质激素类药物的临床应用研究[J].北方药学2019,16(3):172-173.Xiao YM.Clinical application of glucocorticoids[J].Northern Pharm,2019,16(3):172-173.
[14]余玮,胡卫华.解热镇痛药的临床应用和不良反应[J].海峡药学,2007,19(12):100-101.Yu W,Hu WH.Clinical application and adverse reactions of antipyretic analgesics[J].Taiwan Pharm,2007,19(12):100-101.
[15]李婕,丁丽霞,张启明.抗类风湿性关节炎药物不良反应的研究进展[J].药品评价,2006,3(6):442-445.Li J,Ding LX,Zhang QM.Research progress on adverse drug reactions of anti-rheumatoid arthritis drugs[J].Drug Evaluat,2006,3(6):442-445.
[16]池里群,于景娴,高文远.常用治疗类风湿性关节炎药物不良反应的研究进展[J].中国医院用药评价与分析,2015,15(11):1559-1561.Chi LQ,Yu JX,Gao WY.Research progress on adverse drug reactions of commonly used drugs for rheumatoid arthritis[J].Evaluat Anal Drug Use Chin Hospit,2015,15(11):1559-1561.
[17]翁昆,方晨,张亚丽.茶叶标准体系研究[J].中国茶叶加工,2011,(4):14-17.Weng K,Fang C,Zhang YL.Study on tea standard system[J].China Tea Process,2011,(4):14-17.
[18]翁昆,黄皓.论我国茶叶标准体系的建设[J].中国茶叶加工,2009,(3):3-6.Weng K,Huang H.On establishing standard system for tea in China[J].China Tea Process,2009,(3):3-6.
[19]周建良,方翠芬.快速液相色谱-串联质谱联用同时检测抗风湿类中药制剂中13种添加化学药物成分[J].药物分析杂志,2013,33(2):281-285.Zhou JL,Fang CF.Rapid liquid chromatography-tandem mass spectrometry for simultaneous determination of 13 additive chemical components in anti-rheumatic traditional Chinese medicine preparations[J].J Pharm Anal,2013,33(2):281-285.
[20]黎雪清,谭渺.HPLC法快速筛查抗风湿类中成药和保健食品中24种非法添加化学成分[J].中成药,2014,36(9):1891-1894.Li XQ,Tan M.Rapid screening of 24 illegally added chemical constituents in anti-rheumatic Chinese patent medicines and health food by high performance liquid chromatography[J].Chin Patent Med,2014,36(9):1891-1894.
[21]廖瑜.HPLC快速筛查抗风湿类中成药及保健品中非法添加的10种化学药[J].中国现代应用药学,2014,31(7):868-871.Liao Y.Rapid screening of 10 chemicals illegally added in Chinese patent anti-rheumatic drugs and health products by high performance liquid chromatography[J].Mod Appl Pharm China,2014,31(7):868-871.