UPLC-MS/MS同时测定电子烟烟液中安赛蜜等5种合成甜味剂
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摘要
【目的】通过对实验条件的优化,建立了一种测定电子烟烟液中5种人工合成甜味剂(安赛蜜、甜蜜素、糖精钠、阿斯巴甜和纽甜)的超高效液相色谱-串联质谱(UPLC-MS/MS)方法。【方法】样品经超纯水稀释、C18分散固相萃取净化后,以BEH C18色谱柱分离,甲醇-0.1%甲酸水溶液为流动相,外标法定量。【结果】结果表明:①5种甜味剂在0.25～5.0μg/mL的标准工作曲线范围内线性关系良好(r>0.998),检出限(LOD)和定量限(LOQ)分别为0.02～0.05和0.07～0.17 mg·kg-1,回收率为92.5%～105.2%,相对标准偏差(RSDs)<5.0%。②采用该方法对10个电子烟烟液样品进行了检测,1个样品检出甜蜜素,含量为2.48 mg·kg-1,2个样品检出纽甜,含量在3.35～4.52 mg·kg-1之间。【结论】该方法操作简单、快速、灵敏度高、有机溶剂消耗少,适用于电子烟烟液中多种甜味剂的同时检测。
An ultra-high performance liquid chromatography-tandem mass spectrometry(UPLC-MS/MS) method for simultaneous determination of 5 synthetic sweeteners, i.e. Sodium cyclamate, Saccharin sodium, Aspartame, Acesulfame and Neotame, in refill liquids of e-cigarette was developed by optimizing experimental condition. Samples were diluted with ultrapure water and purified by C18. Their extracts were separated on BEH C18 column using methanol-0.1% formic acid as mobile phase. Results were quantified by external standard method.These results showed that: 1) Good linear relation was obtained within the range of standard working solution, with r>0.998. The limits of detection(LODs) and quantification(LOQs) were 0.02～0.05 and 0.07～0.17 mg kg~(-1), respectively. The added standard recoveries of blank samples were within the range of 92.5%～105.2%, with a relative standard deviation less than 5.0%. 2) Ten e-cigarette samples were tested by this method. One sample was detected as cyclamate with a content of 2.48 mg kg~(-1). Two samples were found to contain neotame, with the content between 3.35 and 4.52 mg kg~(-1). The method proposed in this study has the advantages of simple operation, rapid speed, high sensitivity and robustness, which is suitable for simultaneous detection of various sweeteners in refill liquids of electronic cigarette.
An ultra-high performance liquid chromatography-tandem mass spectrometry(UPLC-MS/MS) method for simultaneous determination of 5 synthetic sweeteners, i.e. Sodium cyclamate, Saccharin sodium, Aspartame, Acesulfame and Neotame, in refill liquids of e-cigarette was developed by optimizing experimental condition. Samples were diluted with ultrapure water and purified by C18. Their extracts were separated on BEH C18 column using methanol-0.1% formic acid as mobile phase. Results were quantified by external standard method.These results showed that: 1) Good linear relation was obtained within the range of standard working solution, with r>0.998. The limits of detection(LODs) and quantification(LOQs) were 0.02～0.05 and 0.07～0.17 mg kg~(-1), respectively. The added standard recoveries of blank samples were within the range of 92.5%～105.2%, with a relative standard deviation less than 5.0%. 2) Ten e-cigarette samples were tested by this method. One sample was detected as cyclamate with a content of 2.48 mg kg~(-1). Two samples were found to contain neotame, with the content between 3.35 and 4.52 mg kg~(-1). The method proposed in this study has the advantages of simple operation, rapid speed, high sensitivity and robustness, which is suitable for simultaneous detection of various sweeteners in refill liquids of electronic cigarette.
引文
[1]管莹,高茜,李雪梅,等.电子烟烟液体位毒理学评价用细胞筛选研究[J].中国烟草学报, 2018, 24(5):84-90.GUAN Ying, GAO Qian, LI Xuemei, et al.Screening of cells for in vitro toxicology test of e-liquid[J]. Acta Tabacaria Sinica, 2018, 24(5):84-90.
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[4]杨洋,徐建,刘金莉,等.电子烟液中烟碱稳定性及其释放行为分析[J].中国烟草学报,2017, 23(6):16-21.YANG Yang, XU Jian, LIU Jinli, et al. Stability and release behavior of nicotine in e-liquids[J].Acta Tabacaria Sinica, 2017,23(6):16-21.
[5]丁彩霞,李钢,郑赛晶,等.固相萃取-气相色谱-质谱法分析电子烟烟液中的香味成分[J].分析实验室,2016, 35(7):846-849.DING Caixia, LI Gang, ZHENG Saijin, et al. Analysis of aroma components in E-liquid by solid phase extraction-gas chromatography-mass spectrometry[J]. Chinese Journal of Analysis Laboratory, 2016, 35(7):846-849.
[6]GB2760-2014食品安全国家标准食品添加剂使用标准[S].GB2760-2014 National Food Safety Standard for Uses of Food Additives[S].
[7]武太鹏,马康.合成甜味剂检测技术的研究进展[J].化学分析量,2017, 26(6):109-115.WU Taipeng, MA Kang. Research Development of Detection Technology of Synthetic Sweetener[J].Chemical Analysis and Meterage, 2017, 26(6):109-115.
[8]Chattopadhyay S, Raychaudhuri U, Chakraborty R. Artificial sweeteners-a review[J]. Journal of Food Science and Technology,2014, 51(4):611-621.
[9]Larsen J C. Artificial sweeteners[J].Nutrafoods, 2012, 11(1):3-9.
[10]桂建业,孙威,张辰凌,等.离子色谱-串联质谱法分析环境水体中痕量人工甜味剂[J].分析化学, 2016, 44(3):361-366.GUI Jianye, SUN Wei, ZHANG Chenling, et al. An Innovative Approach to Sensitive Artificial Sweeteners Analysis by Ion Chromatography-Triple Quadrupole Mass Spectrometry[J]. Chinese Journal of Analytical Chemistry, 2016, 44(3):361-366.
[11]Horie M, Ishikawa F, Oishi M, et al. Rapid determination of cyclamate in foods by solid-phase extraction and capillary electrophoresis[J]. Journal of Chromatography A, 2007, 1154(1-2):423-428.
[12]Zhao Y G, Cai M Q, Chen X H, et al. Analysis of nine food additives in wine by dispersive solid-phase extraction and reversedphase high performance liquid chromatography[J]. Food Research International, 2013, 52(1):350-358.
[13]包懿,石金娥,刘斌,等.高效液相色谱/二极管阵列法快速测定白酒、配制酒与葡萄酒中5种人工合成甜味剂[J].分析测试学报. 2017,36(05):674-678.BAO Yi, SHI Jine, LIU Bin, et al. Rapid Determination of Five Artificial Sweeteners in White Spirit, Mixed Liquor and Wine by High Performance Liquid Chromatography/Diode Array Detector[J].Journal of Instrumental Analysis, 2017, 36(05):674-678.
[14]嵇超,冯峰,陈正行,等.高效液相色谱-串联质谱法测定葡萄酒中的5种人工合成甜味剂[J].色谱, 2010, 28(8):749-753.JI Chao, FENG Feng, CHEN Zhengxing, et al. Determination of five synthetic sweeteners in wines using high performance liquid chromatography-tandem mass spectrometry[J]. Chinese Journal of Chromatography, 2010, 28(8):749-753.
[15]刘晓霞,丁利,刘锦霞,等.高效液相色谱-串联质谱法测定食品中6种人工合成甜味剂[J].色谱, 2010, 28(11):1020-1025.LIUXiaoxia,DINGLi,LIUJinxia,etal.Simultaneous determination of six synthetic sweeteners in food by high performance liquid chromatography-tandem mass spectrometry[J].Chinese Journal of Chromatography, 2010, 28(11):1020-1025.
[16]Chang C S, Tai S Y. Detection of 10 sweeteners in various foods by liquid chromatography/tandem mass spectrometry[J]. Journal of Food&Drug Analysis, 2014, 22(3):318-328.
[17]Pawe Kubica, Jacek Namie?nik, Andrzej Wasik. Determination of eight artificial sweeteners and common Stevia rebaudiana glycosides in non-alcoholic and alcoholic beverages by reversedphaseliquidchromatographycoupledwithtandemmass spectrometry[J].Analytical and Bioanalytical Chemistry(2015)407:1505-1512.
[18]李晶,杨叶昆,陈建华,等.超高效液相色谱-串联质谱法测定香精香料中的甜味剂和色素[J].理化检验-化学分册,2015,51(12):1724-1728.LI Jing, YANG Yekun, CHEN Jianhua, et al. Simultaneous Determination of sweeteners and pigments in essences and spices by UHPLC-MS/MS[J].Physical testing and chemical analysis part B:chemical analysis, 2015, 51(12):1724-1728.
[19]李晶,徐济仓,缪明明,等.固相萃取-超高效液相色谱/串联质谱同时检测饮料中13种禁限用食品添加剂[J].分析科学学报, 2013, 29(4):488-492.LI Jing, XU Jicang, MIAO Mingming, et al. Solid phase extractionultra high performance liquid chromatography-tradem mass spectrometry for simulatneous determination of 13 restricted food additives in beverages[J].Journal of analytical science, 2013, 29(4):488-492.
[20]GB/T 27417-2017合格评定化学分析方法确认和验证指[S]. GB/T274147-2017 Comformity assessment-Guidance on valadation and verification of chemical analytical methods[S].
[21]GB/T 32465-2015化学分析方法验证确认和内部质量控制要求[S].GB/T 32465-2015 Requierment for verification validation of detection methods and internal quality control on chemical analysis[S].
[2]樊美娟,赵乐,崔华鹏,等.电子烟中化学成分风险研究进展[J].中国烟草学报, 2018, 24(3):120-129.FAN Meijuan, ZHAO Le, CUI Huapeng, et al. Research advances in risk evaluation of chemical components associated with e-cigarettes[J]. Acta Tabacaria Sinica, 2018, 24(3):120-129.
[3]李磊,周宁波,屈湘辉.新型烟草制品市场发展及法律监管[J].中国烟草学报, 2018, 24(2):100-110.LI Lei, ZHOU Ningbo, QU Xianghui. Market development and regulation of novel tobacco products[J]. Acta Tabacaria Sinica,2018, 24(2):100-110.
[4]杨洋,徐建,刘金莉,等.电子烟液中烟碱稳定性及其释放行为分析[J].中国烟草学报,2017, 23(6):16-21.YANG Yang, XU Jian, LIU Jinli, et al. Stability and release behavior of nicotine in e-liquids[J].Acta Tabacaria Sinica, 2017,23(6):16-21.
[5]丁彩霞,李钢,郑赛晶,等.固相萃取-气相色谱-质谱法分析电子烟烟液中的香味成分[J].分析实验室,2016, 35(7):846-849.DING Caixia, LI Gang, ZHENG Saijin, et al. Analysis of aroma components in E-liquid by solid phase extraction-gas chromatography-mass spectrometry[J]. Chinese Journal of Analysis Laboratory, 2016, 35(7):846-849.
[6]GB2760-2014食品安全国家标准食品添加剂使用标准[S].GB2760-2014 National Food Safety Standard for Uses of Food Additives[S].
[7]武太鹏,马康.合成甜味剂检测技术的研究进展[J].化学分析量,2017, 26(6):109-115.WU Taipeng, MA Kang. Research Development of Detection Technology of Synthetic Sweetener[J].Chemical Analysis and Meterage, 2017, 26(6):109-115.
[8]Chattopadhyay S, Raychaudhuri U, Chakraborty R. Artificial sweeteners-a review[J]. Journal of Food Science and Technology,2014, 51(4):611-621.
[9]Larsen J C. Artificial sweeteners[J].Nutrafoods, 2012, 11(1):3-9.
[10]桂建业,孙威,张辰凌,等.离子色谱-串联质谱法分析环境水体中痕量人工甜味剂[J].分析化学, 2016, 44(3):361-366.GUI Jianye, SUN Wei, ZHANG Chenling, et al. An Innovative Approach to Sensitive Artificial Sweeteners Analysis by Ion Chromatography-Triple Quadrupole Mass Spectrometry[J]. Chinese Journal of Analytical Chemistry, 2016, 44(3):361-366.
[11]Horie M, Ishikawa F, Oishi M, et al. Rapid determination of cyclamate in foods by solid-phase extraction and capillary electrophoresis[J]. Journal of Chromatography A, 2007, 1154(1-2):423-428.
[12]Zhao Y G, Cai M Q, Chen X H, et al. Analysis of nine food additives in wine by dispersive solid-phase extraction and reversedphase high performance liquid chromatography[J]. Food Research International, 2013, 52(1):350-358.
[13]包懿,石金娥,刘斌,等.高效液相色谱/二极管阵列法快速测定白酒、配制酒与葡萄酒中5种人工合成甜味剂[J].分析测试学报. 2017,36(05):674-678.BAO Yi, SHI Jine, LIU Bin, et al. Rapid Determination of Five Artificial Sweeteners in White Spirit, Mixed Liquor and Wine by High Performance Liquid Chromatography/Diode Array Detector[J].Journal of Instrumental Analysis, 2017, 36(05):674-678.
[14]嵇超,冯峰,陈正行,等.高效液相色谱-串联质谱法测定葡萄酒中的5种人工合成甜味剂[J].色谱, 2010, 28(8):749-753.JI Chao, FENG Feng, CHEN Zhengxing, et al. Determination of five synthetic sweeteners in wines using high performance liquid chromatography-tandem mass spectrometry[J]. Chinese Journal of Chromatography, 2010, 28(8):749-753.
[15]刘晓霞,丁利,刘锦霞,等.高效液相色谱-串联质谱法测定食品中6种人工合成甜味剂[J].色谱, 2010, 28(11):1020-1025.LIUXiaoxia,DINGLi,LIUJinxia,etal.Simultaneous determination of six synthetic sweeteners in food by high performance liquid chromatography-tandem mass spectrometry[J].Chinese Journal of Chromatography, 2010, 28(11):1020-1025.
[16]Chang C S, Tai S Y. Detection of 10 sweeteners in various foods by liquid chromatography/tandem mass spectrometry[J]. Journal of Food&Drug Analysis, 2014, 22(3):318-328.
[17]Pawe Kubica, Jacek Namie?nik, Andrzej Wasik. Determination of eight artificial sweeteners and common Stevia rebaudiana glycosides in non-alcoholic and alcoholic beverages by reversedphaseliquidchromatographycoupledwithtandemmass spectrometry[J].Analytical and Bioanalytical Chemistry(2015)407:1505-1512.
[18]李晶,杨叶昆,陈建华,等.超高效液相色谱-串联质谱法测定香精香料中的甜味剂和色素[J].理化检验-化学分册,2015,51(12):1724-1728.LI Jing, YANG Yekun, CHEN Jianhua, et al. Simultaneous Determination of sweeteners and pigments in essences and spices by UHPLC-MS/MS[J].Physical testing and chemical analysis part B:chemical analysis, 2015, 51(12):1724-1728.
[19]李晶,徐济仓,缪明明,等.固相萃取-超高效液相色谱/串联质谱同时检测饮料中13种禁限用食品添加剂[J].分析科学学报, 2013, 29(4):488-492.LI Jing, XU Jicang, MIAO Mingming, et al. Solid phase extractionultra high performance liquid chromatography-tradem mass spectrometry for simulatneous determination of 13 restricted food additives in beverages[J].Journal of analytical science, 2013, 29(4):488-492.
[20]GB/T 27417-2017合格评定化学分析方法确认和验证指[S]. GB/T274147-2017 Comformity assessment-Guidance on valadation and verification of chemical analytical methods[S].
[21]GB/T 32465-2015化学分析方法验证确认和内部质量控制要求[S].GB/T 32465-2015 Requierment for verification validation of detection methods and internal quality control on chemical analysis[S].