ICP-MS法测定消渴清颗粒原料药材中15种重金属和有害元素及其不确定度评估
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摘要
目的:建立电感耦合等离子体质谱法(ICP-MS法)测定消渴清颗粒的5种原料药材苍术、蒲黄、知母、黄连和地锦草中15种重金属及有害元素含量,并对测定结果进行不确定度评估。方法:采用ICP-MS(KED模式)联合微波消解法,分析测定流程,建立数学模型,根据JJF1059.1-2012《测量不确定度的评定与表示》对测量结果的各不确定度来源进行分析和评估,并计算合成不确定度。结果:实验建立的15种重金属及有害元素检测方法具有良好的线性关系,且重复性和精确度良好,线性系数均大于0.992,RSD低于5.0%,加样回收率在87%～115%之间。其不确定度主要来源于曲线拟合和微波消解过程。15种重金属及有害元素含量的合成不确定度分别为V 2.93%,Cr 4.43%,Ni 2.65%,Cu 5.70%,As 6.92%,Mo 2.02%,Ru 1.76%,Rh 2.07%,Pd9.39%,Cd 2.75%,Os 4.72%,Ir 1.41%,Pt 7.31%,Hg 3.29%,Pb 4.28%。结论:ICP-MS法对消渴清颗粒原料药材中15种重金属及有害元素的测量中,可通过优化曲线拟合及微波消解过程从而减小不确定度的值。
Objective:To establish a determination method of fifteen kinds of heavy metals and harmful elements in five raw materials(Atractylodis Rhizoma,Typhae Pollen,Anemarrhenae Rhizoma,Coptidis Rhizoma and Euphorbiae Humifusae Herba) of Xiaokeqing granules by ICP-MS,and to analyze the uncertainty.Methods:The microwave digest technique combined with ICP-MS(KED mode) was used to determinate the 15 kinds of heavy metals and harmful elements.Through establishment of the mathematical model,the main sources of the uncertainty resulted from the determination process were calculated and discussed by the method recommended by JJF1059.1-2012 ‘Evaluation and expression of uncertainty in measurement'.Results:The detection methods of 15 heavy metals and harmful elements established in the experiment had good linear relationship,good repeatability and accuracy.The linear coefficients were greater than 0.992 with RSDs less than 5.0%,and the recovery rates were between 87% and 115%.The uncertainty sources were mainly from the curve fitting and microwave digestion process.The uncertainties of the measurement by ICP-MS were 2.93% for V,4.43% for Cr,2.65% for Ni,5.70%for Cu,6.92% for As,2.02% for Mo,1.76% for Ru,2.07% for Rh,9.39% for Pd,2.75% for Cd,4.72% for Os,1.41% for Ir,7.31% for Pt,3.29% for Hg and 4.28% for Pb.Conclusion:The uncertainties of fifteen kinds of heavy metals and harmful elements in five raw materials of Xiaokeqing granules determined by ICP-MS can be reduced by optimization of the curve fitting and microwave digestion process.
Objective:To establish a determination method of fifteen kinds of heavy metals and harmful elements in five raw materials(Atractylodis Rhizoma,Typhae Pollen,Anemarrhenae Rhizoma,Coptidis Rhizoma and Euphorbiae Humifusae Herba) of Xiaokeqing granules by ICP-MS,and to analyze the uncertainty.Methods:The microwave digest technique combined with ICP-MS(KED mode) was used to determinate the 15 kinds of heavy metals and harmful elements.Through establishment of the mathematical model,the main sources of the uncertainty resulted from the determination process were calculated and discussed by the method recommended by JJF1059.1-2012 ‘Evaluation and expression of uncertainty in measurement'.Results:The detection methods of 15 heavy metals and harmful elements established in the experiment had good linear relationship,good repeatability and accuracy.The linear coefficients were greater than 0.992 with RSDs less than 5.0%,and the recovery rates were between 87% and 115%.The uncertainty sources were mainly from the curve fitting and microwave digestion process.The uncertainties of the measurement by ICP-MS were 2.93% for V,4.43% for Cr,2.65% for Ni,5.70%for Cu,6.92% for As,2.02% for Mo,1.76% for Ru,2.07% for Rh,9.39% for Pd,2.75% for Cd,4.72% for Os,1.41% for Ir,7.31% for Pt,3.29% for Hg and 4.28% for Pb.Conclusion:The uncertainties of fifteen kinds of heavy metals and harmful elements in five raw materials of Xiaokeqing granules determined by ICP-MS can be reduced by optimization of the curve fitting and microwave digestion process.
引文
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[11]刘长姣,王磊,刘长龙,等.ICP-MS法测定人参中Pb含量的不确定度评定[J].中国食品添加剂,2017(6):200LIU CJ,WANG L,LIU CL,et al.Uncertainty evaluation for determining concentration of Pb in Ginseng by ICP-MS[J].China Food Add,2017(6):200
[12]HE MY,LU H,LUO CG,et al.Determining trace metal elements in the tooth enamel from Hui and Han Ethnic groups in China using microwave digestion and inductively coupled plasma mass spectrometry(ICP-MS)[J].Microchem J,2016,127:142
[13]王露黔,王旭,佟玲,等.消渴清颗粒UPLC-PDA-ELSD指纹图谱的建立及5个主要成分的测定[J].中草药,2013,44(24):3482WANG LQ,WANG X,TONG L,et al.Establishment of UPLC-PDA-ELSD fingerprints of Xiaokeqing granules and determination of its five main constituents[J].Chin Tradit Herb Drugs,2013,44(24):3482
[14]王枚博,夏晶,王欣美,等.金银花等10种中药材中15种无机元素分布规律及其相关性研究[J].中国药学杂志,2012,47(8):620WANG MB,XIA J,WANG XM,et al.Study on distribution and correlation of fifteen inorganic elements in ten kinds of Chinese medicinal materials[J].Chin Pharm J,2012,47(8):620
[2]洪薇,赵静,李绍平.中药重金属限量控制现状与对策[J].药物分析杂志,2007,27(11):1849HONG W,ZHAO J,LI SP.Strategies and current status on limit control of heavy metals in traditional Chinese medicine[J].Chin JPharm Anal,2007,27(11):1849
[3]ROCHA SRDL,SáNCHEZ-MUNIZ FJ,GóMEZ-JUARISTI M,et al.Trace elements determination in edible seaweeds by an optimized and validated ICP-MS method[J].J Food Composit Anal,2009,22(4):330
[4]孙少杰,韩红玉,王光辉.电感耦合等离子体质谱及其技术研究进展[J].山西化工,2015,35(3):46SUN SJ,HAN HY,WANG GH.Inductively coupled plasma mass spectrometry and its technology research[J].Shanxi Chem Ind,2015,35(3):46
[5]胡坪,罗国安,赵中振,等.中药材定量分析中测量不确定度的评定方法及其影响因素的研究[J].药物分析杂志,2005,25(4):455HU P,LUO GA,ZHAO ZZ,et al.Study on the evaluating method and the affecting factors of measurement uncertainty for the determination of marker compounds in Chinese materia medica[J].Chin J Pharm Anal,2005,25(4):455
[6]陈佳,乔菲,金红宇,等.ICP-MS法测定马钱子中重金属及有害元素含量的不确定度评定[J].药物分析杂志,2013,33(12):2176CHEN J,QIAO F,JIN HY,et al.Evaluation of the uncertainty for the determination of heavy metals in Strychni Semen by ICP-MS[J].Chin J Pharm Anal,2013,33(12):2176
[7]国家质量技术监督局.JJF1059-1999测量不确定度评定与表示[M].北京:中国计量出版社,1999:1574The State Bureau of Quality and Technical Supervision.JJF1059-1999 Evaluation and Expression of Uncertainty in Measurement[M].Beijing:China Metrology Publishing House,1999:1574
[8]中国实验室国家认可委员会.CNAS-GL06-2006化学分析中不确定度的评估指南[M].北京:中国计量出版社,2006:31China National Accreditation Board for Laboratory.CNAS-GL06-2006 Guidance on Evaluating the Uncertainty in Chemical Analysis[M].Beijing:China Metrology Publishing House,2006:31
[9]国家质量技术监督局.JJF1059.1测量不确定度评定与表示[M].北京:中国计量出版社,2012:4The State Bureau of Quality and Technical Supervision.JJF 1059.1Evaluation and Expression of Uncertainty in Measurement[M].Beijing:China Metrology Publishing House,2012:4
[10]国家质量技术监督局.JJG196常用玻璃容器检定规程[M].北京:中国计量出版社,2006:6The State Bureau of Quality and Technical Supervision.JJG196Verification Regulation of Working Glass Container[M].Beijing:China Metrology Publishing House,2006:6
[11]刘长姣,王磊,刘长龙,等.ICP-MS法测定人参中Pb含量的不确定度评定[J].中国食品添加剂,2017(6):200LIU CJ,WANG L,LIU CL,et al.Uncertainty evaluation for determining concentration of Pb in Ginseng by ICP-MS[J].China Food Add,2017(6):200
[12]HE MY,LU H,LUO CG,et al.Determining trace metal elements in the tooth enamel from Hui and Han Ethnic groups in China using microwave digestion and inductively coupled plasma mass spectrometry(ICP-MS)[J].Microchem J,2016,127:142
[13]王露黔,王旭,佟玲,等.消渴清颗粒UPLC-PDA-ELSD指纹图谱的建立及5个主要成分的测定[J].中草药,2013,44(24):3482WANG LQ,WANG X,TONG L,et al.Establishment of UPLC-PDA-ELSD fingerprints of Xiaokeqing granules and determination of its five main constituents[J].Chin Tradit Herb Drugs,2013,44(24):3482
[14]王枚博,夏晶,王欣美,等.金银花等10种中药材中15种无机元素分布规律及其相关性研究[J].中国药学杂志,2012,47(8):620WANG MB,XIA J,WANG XM,et al.Study on distribution and correlation of fifteen inorganic elements in ten kinds of Chinese medicinal materials[J].Chin Pharm J,2012,47(8):620