保健食品中非法添加药物的广谱筛查和确证
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摘要
采用液相色谱仪—二极管阵列检测器-离子阱-飞行时间串联质谱仪(LCMS-DAD-IT-TOF)建立减肥类非法添加药物高分辨质谱数据库。样品经乙腈超声提取,提取液经QuEChERS吸附剂净化,以ZORBAX Eclipse AAA色谱柱(150mm×4.6 mm,4.5μm)分离,乙腈和0.1%乙酸为流动相梯度洗脱。筛查限为0.10~0.75 mg/kg,平均回收率在49.4%~88.1%;相对标准偏差为5.0~14.8%。该方法通过紫外光谱确定非法添加药物特征吸收波长,结合滥用药物高分辨质谱数据库,通过精确质量数的检索匹配对非法添加药物实现快速筛查,并使用保留时间、同位素丰度和多级特征碎片离子进行确证。根据多级碎片离子,推导出裂解途径。具有简便、快速、高效、准确等优点。在缺乏标准品或对照品的情况下,即可得到准确可靠的结论。适用于保健食品中非法添加药物的有效快速筛查。
The high resolution mass spectrometry database of weightloss illegally added drugs was established base on liquid chromatography-diode array detector-ion trap-time of flight tandem mass spectrometry(LC-DAD-MS-IT-TOF).The analytes in samples were extracted with acetonitrile and the extract was purified with the mixed QuEChERS sorbents.In the chromatographic analysis,target compounds were separated on a ZORBAX Eclipse AAA column(150 mm × 4.6 mm,4.5μm)with the gradient elution using the mobile phases of acetonitrile and water containing 0.1% acetic acid.The results showed that the screening detection limit(SDL)of the target compounds were ranged from 0.10~0.75 mg/kg.The method validation was carried out at SDL levels,and the recoveries were 49.4%~88.1%.with the relative standard deviations(RSDs)of 5.0% ~14.8%.The characteristic absorption wavelength of illegally added drugs was determined by UV spectrum.The screening of analytes was performed by precision mass matching and library searching.The retention time,isotopic abundance and multiple-stage ion mass spectral was employed to the confirmation.Moreover,the ion fragmentation patterns of these drugs can be exploited to predict the chemical formula and the fragmentation pathway.This method is simple,fast,credible and high sensitivity,which can be applied to simultaneous screening and identification of illegally added drugs in health foods.
The high resolution mass spectrometry database of weightloss illegally added drugs was established base on liquid chromatography-diode array detector-ion trap-time of flight tandem mass spectrometry(LC-DAD-MS-IT-TOF).The analytes in samples were extracted with acetonitrile and the extract was purified with the mixed QuEChERS sorbents.In the chromatographic analysis,target compounds were separated on a ZORBAX Eclipse AAA column(150 mm × 4.6 mm,4.5μm)with the gradient elution using the mobile phases of acetonitrile and water containing 0.1% acetic acid.The results showed that the screening detection limit(SDL)of the target compounds were ranged from 0.10~0.75 mg/kg.The method validation was carried out at SDL levels,and the recoveries were 49.4%~88.1%.with the relative standard deviations(RSDs)of 5.0% ~14.8%.The characteristic absorption wavelength of illegally added drugs was determined by UV spectrum.The screening of analytes was performed by precision mass matching and library searching.The retention time,isotopic abundance and multiple-stage ion mass spectral was employed to the confirmation.Moreover,the ion fragmentation patterns of these drugs can be exploited to predict the chemical formula and the fragmentation pathway.This method is simple,fast,credible and high sensitivity,which can be applied to simultaneous screening and identification of illegally added drugs in health foods.
引文
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[8]林艳萍,司端运,刘昌孝.液质联用分析中药降糖制剂中掺入的西药成分[J].天津大学学报,2008,41(6):720-724.
[9]杨钊,陈安珍,吴爱英,等.UPLC-MS/MS测定降糖类中成药及保健品中11种化学药[J].药物分析杂志,2009,29(12):2 127-2 130.
[10]王美玲,曾乐,颜鸿飞,等.高效液相色谱-离子阱飞行时间串联质谱法快速筛查保健食品中非法添加的磷酸二酯酶-5抑制剂及其类似物[J].分析测试学报,2014,33(3):239-247.
[11]张帆,颜鸿飞,戴洁云,等.食品多组分添加剂及非法添加物的HPLC-HRMS广谱筛查[J].食品与机械,2016,32(8):42-48,62.
[12]SONG Fen-hong,MONROE Douglas,EL-DEMERDSH Aref,et al.Screening for multiple weight loss and related drugs in dietary supplement materials by flow injection tandem mass spectrometry and their confirmation by liquid chromatography tandem mass spectrometry[J].Pharmaceutical and Biomedical Analysis,2014,88:136-143.
[2]刘吉金,李军.减肥食品或保健品中非法添加盐酸西布曲明、盐酸芬氟拉明、酚酞的快速检测方法研究[J].药物分析杂志,2006,26(6):793-794.
[3]张喆,高青,余倩,等.中药制剂及保健品中违禁添加9种化学降糖药HPLC-MS/MS定性检测[J].中国医药工业杂志,2007,38(1):38-43.
[4]张平,黄赵刚,程钢,等.降糖宁胶囊中掺有西药降糖成分的检测[J].安徽医药,2006,10(3):48.
[5]宋家玉,周景洋,丰硕,等.薄层色谱法检测降糖中药制品中的格列本脲[J].中国卫生检验杂志,2006,16(11):1 339-1 3401.
[6]杨蕾,谢华,黄瑛,等.HPLC法测定格列美脲胶囊中格列美脲的含量[J].中国药品标准,2002,3(6):59.
[7]李丹,文红梅,崔福春,等.LC-MS/MS法快速测定中成药、保健食品中非法添加的36种化学成分[J].药物分析杂志,2010,30(8):1 527-1 532.
[8]林艳萍,司端运,刘昌孝.液质联用分析中药降糖制剂中掺入的西药成分[J].天津大学学报,2008,41(6):720-724.
[9]杨钊,陈安珍,吴爱英,等.UPLC-MS/MS测定降糖类中成药及保健品中11种化学药[J].药物分析杂志,2009,29(12):2 127-2 130.
[10]王美玲,曾乐,颜鸿飞,等.高效液相色谱-离子阱飞行时间串联质谱法快速筛查保健食品中非法添加的磷酸二酯酶-5抑制剂及其类似物[J].分析测试学报,2014,33(3):239-247.
[11]张帆,颜鸿飞,戴洁云,等.食品多组分添加剂及非法添加物的HPLC-HRMS广谱筛查[J].食品与机械,2016,32(8):42-48,62.
[12]SONG Fen-hong,MONROE Douglas,EL-DEMERDSH Aref,et al.Screening for multiple weight loss and related drugs in dietary supplement materials by flow injection tandem mass spectrometry and their confirmation by liquid chromatography tandem mass spectrometry[J].Pharmaceutical and Biomedical Analysis,2014,88:136-143.