液相色谱-四级杆-静电轨道阱高分辨质谱法测定保健食品中降压类药物
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摘要
目的建立一种液相色谱-四级杆-高分辨质谱仪测定保健食品中11种降压类药物的分析方法。方法采用甲醇-水混合溶液超声提取,滤膜过滤,采用0.1%甲酸和乙腈作为流动相进行梯度洗脱,质谱(ESI+)采用全扫描(fullscan)+数据依赖MS2(ddMS2)检测模式对降压类药物进行监测,根据母离子及子离子精确质量数进行定性与定量分析。结果 11种降压药分离完全,线性范围均为2.0～100μg/L,相关系数(r~)均不低于0.9915,平均回收率为72.4%～97.1%,相对标准偏差为5.0%～13.9%,液体类样品定量限为0.5～2.5μg/kg,固体类样品定量限为2.5～12.5μg/kg。结论该方法快速、灵敏,适合测定保健食品中降压类药物。
Objective To establish a method for determination of 11 kinds of antihypertensive drugs in health food by liquid chromatography-quadrupole-orbitrap high resolution mass spectrometry(LC-Q-Orbitrap). Methods The antihypertensive drugs in samples were extracted by ultrasound extraction with methanol-water mixed solvent,and determined after filtration with membrane. The drugs were separated on a reversed phase column using a gradient elution program of 0.1% formic acid aqueous solution and acetonitrile. The LC-Q-Orbitrap(ESI+) with fullscan and data dependency MS2(ddMS2) was used, and identification of the 11 kinds of antihypertensive drugs was performed based upon the exact mass of mother ion and product ion. Results The 11 kinds of antihypertensive drugs were completely separated with a linear range of 2.0 to 100 μg/L. The correlation coefficients(r~2) were not less than0.9915. The average recoveries were from 72.4% to 97.1% and the relative standard deviations were from 5.0% to13.9%. The limits of quantitation(LOQs) of liquid samples were from 0.5 to 2.5 μg/kg, and those of solid samples were from 2.5 to 12.5 μg/kg. Conclusion This method is rapid and sensitive, which is suitable for determination of antihypertensive drugs in health food.
Objective To establish a method for determination of 11 kinds of antihypertensive drugs in health food by liquid chromatography-quadrupole-orbitrap high resolution mass spectrometry(LC-Q-Orbitrap). Methods The antihypertensive drugs in samples were extracted by ultrasound extraction with methanol-water mixed solvent,and determined after filtration with membrane. The drugs were separated on a reversed phase column using a gradient elution program of 0.1% formic acid aqueous solution and acetonitrile. The LC-Q-Orbitrap(ESI+) with fullscan and data dependency MS2(ddMS2) was used, and identification of the 11 kinds of antihypertensive drugs was performed based upon the exact mass of mother ion and product ion. Results The 11 kinds of antihypertensive drugs were completely separated with a linear range of 2.0 to 100 μg/L. The correlation coefficients(r~2) were not less than0.9915. The average recoveries were from 72.4% to 97.1% and the relative standard deviations were from 5.0% to13.9%. The limits of quantitation(LOQs) of liquid samples were from 0.5 to 2.5 μg/kg, and those of solid samples were from 2.5 to 12.5 μg/kg. Conclusion This method is rapid and sensitive, which is suitable for determination of antihypertensive drugs in health food.
引文
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[12]凌海燕,汤燕,朱宁,等.HPLC-Q-TOF-MS/MS法检测降压类中成药中非法添加的24种化学物质[J].中国药房,2016,27(33):4712-4715.Ling HY,Tang Y,Zhu N,et al.Detection of 24 chemical substances that illegally added into antihypertensive traditional Chinese patent medicines by HPLC-Q-TOF-MS/MS[J].China Pharm,2016,27(33):4712-4715.
[13]巩丽萍,田晨颖,郭常川,等.超高效液相色谱-四极杆/静电场轨道阱高分辨质谱快速筛查及定量分析中成药或保健品中非法添加的24种消炎止痛类化学成分[J].中国药学杂,2015,50(24):2154-2159.Gong LP,Tian CY,Guo CC,et al.Rapid screening and quantitative detection of 24 illegally added anti-inflammatory painkillers in traditional Chinese medicines and health foods by ultra performance liquid chromatography-quadrupole/electrostaticfield orbitrap high resolution mass spectrometry[J].Chin Pharm J,2015,50(24):2154-2159.
[14]杜彦山,李强,吴春敏,等.超高效液相色谱-四极杆/静电场轨道阱高分辨质谱快速筛查及定量分析保健品中11种非法添加降糖药物[J].色谱,2015,33(4):371-376.Du YS,Li Q,Wu CM,et al.Rapid screening and quantitative detection of11 illegally added antidiabetics in health care products by ultra performance liquid chromatography-quadrupole/electrostatic field orbitrap high resolution mass spectrometry[J].Chin J Chromatogr,2015,33(4):371-376.
[15]张晓光,李强,孙磊,等.超高效液相色谱-静电场轨道阱高分辨质谱快速筛查保健品中23种非法添加西药成分[J].食品科学,2015,36(14):187-191.Zhang XG,Li Q,Sun L,et al.Rapid screening and confirmation of 23illicit western medicine components in health food products by ultra high performance liquid chromatography-orbitrap high resolution mass spectrometry[J].Food Sci,2015,36(14):187-191.
[16]董喆,李梦怡,吴迪,等.超高效液相色谱-四极杆/静电场轨道阱高分辨质谱法快速筛查及定量分析减肥类保健品中20种非法添加药物[J].食品安全质量检测学报,2017,8(10):4031-4038.Dong Z,Li MY,Wu D,et al.Rapid screening and quantitative detection of20 kinds of illegally added drugs in diet health foods by ultra performance liquid chromatography-quadrupole/electrostatic field orbitrap high resolution mass spectrometry[J].J Food Saf Qual,2017,8(10):4031-4038.
[2]国家食品药品监督管理局.药品检验补充检验方法和检验项目批准件(编号:2009032)[S].China Food and Drug Administration.Inspection and additional testing methods and project approval documents(No.2009032)[S].
[3]王铁松,仝禹,郑洁,等.薄层色谱法快速筛查降脂、降压、止咳平喘类中药制剂中的29种添加化学药物[J].中国药学杂志,2016,45(11):857-861.Wang TS,Tong Y,Zheng J,et al.Detection of 29 adulterations in lipid-regulating,antihypertensive,antitussive and antiasthmatic herbal remedies by TLC[J].Chin Pharm J,2016,45(11):857-861.
[4]董晶晶,郝翔.激光拉曼光谱法测定中药三七花中非法添加的化学降压药[J].中国药师,2017,20(2):391-393.Dong JJ,Hao X.Identification of hypotensive drugs illegally added to flower buds of panax notoginseng by laser Raman spectroscopy[J].China Pharm,2017,20(2):391-393.
[5]刘吉金,杨敏,李军,等.HPLC同时检测保健品及中成药中非法添加9种抗高血压化学药物的研究[J].中国现代应用药学杂志,2008,25(8):717-719.Liu JJ,Yang M,Li J,et al.Study on the method for separation and identification of 9 antihypertensives by HPLC[J].Chin J Mod Appl Pharm,2008,25(8):717-719.
[6]陈惠玲,封令霞.HPLC检测中药中非法添加化学降压药物[J].中国现代应用药学,2011,28(13):1346-1348.Chen HL,Feng LX.Detection of antihypertensive agents illegally added in traditional Chinese medicine by HPLC[J].Chin J Mod Appl Pharm,2011,28(13):1346-1348.
[7]陈国权,黄文静,蔡霞,等.高效液相色谱法测定降压类健康产品中非法添加的4种化学成分[J].中南药学,2018,16(1):107-110.Chen GQ,Huang WJ,Cai X,et al.HPLC determination of 4 illegal chemicals in health products for hypertension[J].Central South Pharm,2018,16(1):107-110.
[8]金舒,杨敏智,申兰慧.HPLC-DAD法同时测定降压类保健食品中非法添加的12种化学成分[J].药学与临床研究,2019,27(1):25-28.Jin S,Yang MZ,Shen LH.Simultaneous determination of twelve Chemical material illegally added in antihypertensive health products by HPLC-DAD[J].Pharm Clin Res,2019,27(1):25-28.
[9]鲁艺,邱颖姮,陈平平,等.降压类保健食品及中成药中添加化学药品的液相色谱-质谱联用测定方法研究[J].药物分析杂志,2010,30(10):1913-1917.Lu Y,Qiu YH,Chen PP,et al.Detection of chemical composition mixed into health care food and traditional Chinese medicine antihypertensive preparations by the liquid chromatography-quadrupole mass spectrometry method[J].Chin J Pharm Anal,2010,30(10):1913-1917.
[10]孙晶,曹玲,冯有龙,等.液质联用法筛查降压类中成药和保健食品中添加的54种化学药物[J].药物分析杂志,2018,38(11):1981-1993.Sun J,Cao L,Feng YL,et al.Screening of 54 illegally added chemical drugs in anti-hypertensive Chinese traditional patent medicine and health foods by liquid chromatography tandem mass spectrometry[J].Chin JPharm Anal,2018,38(11):1981-1993.
[11]王琤帅,舒展,朱洁,等.中成药和保健食品中18种非法添加降压药物的HPLC-QTOF/MS定性检测[J].中国药师,2016,19(6):1084-1087.Wang ZS,Shu Z,Zhu J,et al.Detection of 18 antihypertensive agents illegally added in traditional Chinese medicines and healthy care products by HPLC-QTOF/MS[J].China Pharm,2016,19(6):1084-1087.
[12]凌海燕,汤燕,朱宁,等.HPLC-Q-TOF-MS/MS法检测降压类中成药中非法添加的24种化学物质[J].中国药房,2016,27(33):4712-4715.Ling HY,Tang Y,Zhu N,et al.Detection of 24 chemical substances that illegally added into antihypertensive traditional Chinese patent medicines by HPLC-Q-TOF-MS/MS[J].China Pharm,2016,27(33):4712-4715.
[13]巩丽萍,田晨颖,郭常川,等.超高效液相色谱-四极杆/静电场轨道阱高分辨质谱快速筛查及定量分析中成药或保健品中非法添加的24种消炎止痛类化学成分[J].中国药学杂,2015,50(24):2154-2159.Gong LP,Tian CY,Guo CC,et al.Rapid screening and quantitative detection of 24 illegally added anti-inflammatory painkillers in traditional Chinese medicines and health foods by ultra performance liquid chromatography-quadrupole/electrostaticfield orbitrap high resolution mass spectrometry[J].Chin Pharm J,2015,50(24):2154-2159.
[14]杜彦山,李强,吴春敏,等.超高效液相色谱-四极杆/静电场轨道阱高分辨质谱快速筛查及定量分析保健品中11种非法添加降糖药物[J].色谱,2015,33(4):371-376.Du YS,Li Q,Wu CM,et al.Rapid screening and quantitative detection of11 illegally added antidiabetics in health care products by ultra performance liquid chromatography-quadrupole/electrostatic field orbitrap high resolution mass spectrometry[J].Chin J Chromatogr,2015,33(4):371-376.
[15]张晓光,李强,孙磊,等.超高效液相色谱-静电场轨道阱高分辨质谱快速筛查保健品中23种非法添加西药成分[J].食品科学,2015,36(14):187-191.Zhang XG,Li Q,Sun L,et al.Rapid screening and confirmation of 23illicit western medicine components in health food products by ultra high performance liquid chromatography-orbitrap high resolution mass spectrometry[J].Food Sci,2015,36(14):187-191.
[16]董喆,李梦怡,吴迪,等.超高效液相色谱-四极杆/静电场轨道阱高分辨质谱法快速筛查及定量分析减肥类保健品中20种非法添加药物[J].食品安全质量检测学报,2017,8(10):4031-4038.Dong Z,Li MY,Wu D,et al.Rapid screening and quantitative detection of20 kinds of illegally added drugs in diet health foods by ultra performance liquid chromatography-quadrupole/electrostatic field orbitrap high resolution mass spectrometry[J].J Food Saf Qual,2017,8(10):4031-4038.