酸辅助分散液液微萃取-高效液相色谱-串联质谱法测定果汁中多种真菌毒素
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摘要
建立了酸辅助分散液液微萃取结合高效液相色谱-串联质谱法检测果汁中黄曲霉毒素B_1(AflatoxinB_1,AFB_1)、黄曲霉毒素B_2(Aflatoxin B_2,AFB_2)、黄曲霉毒素G_1(Aflatoxin G_1,AFG_1)、黄曲霉毒素G_2(Aflatoxin G_2,AFG_2)、赭曲霉毒素(Ochratoxin A,OTA)、桔霉素(Citrinin,CIT)、链格孢霉酚(Alternariol,AOH)和链格孢甲醚(Alternariol monomethyl Ether,AME)共8种真菌毒素的分析方法。考察了萃取剂的种类以及用量、分散剂用量、平衡体系pH值对萃取效率的影响,获得了最佳的分散液液微萃取(Dispersive liquid-liquid microextraction,DLLME)条件:萃取剂为三氯苯胺,用量为60μL;分散剂为HCl溶液,用量为1500μL;平衡体系pH=5。结果表明,8种真菌毒素在1～500μg/L范围内呈良好的线性关系,相关系数>0.994;在芒果、菠萝和火龙果果汁中的检出限分别为0.15～17.71 ng/L、0.09～7.08 ng/L和0.40～14.29 ng/L;当添加浓度为0.2、1.0和10.0μg/L时,回收率在75.6%～110.0%之间,相对标准偏差<15.5%。本方法简单、快速,有机溶剂用量少,灵敏度高,重现性好,可用于果汁中多种痕量真菌毒素的检测。
A simple and novel sample pretreatment method for determination of eight kinds of mycotoxin in juice samples has been developed using acid-assisted dispersive liquid-liquid microextraction coupled with high performance liquid chromatography-tandem mass spectrometry. The factors effecting extraction efficiency were investigated including the type and volume of extraction solvent,the volume of dispersive solvent and pH of the equilibrium system. Under the optimum extraction conditions including 60 μL of trichloroaniline as extraction solvent,1500 μL of hydrochloric acid solution as dispersive solvent and pH 5 as the acidity of equilibrium system,the method showed a good linearity for these mycotoxins within the concentration range from 1 to 500 μg/L with correlation coefficients higher than 0. 994. The detection limits were 0. 15-17. 71 ng/L,0.09-7.08 ng/L and 0. 40-14. 29 ng/L in fruit juice of mango,pineapple and dragon,respectively. The average recoveries of eight kinds of mycotoxins ranged from 75.6% to 110.0% at three spiked concentrations of 0.2 μg/L,1.0 μg/L and 10.0 μg/L,with the relative standard deviation of lower than 15.5%. The proposed method is simple,fast with less consumption of organic solvent,and has high sensitivity and repeatability,which is suitable for the detection of mycotoxins residues in fruit juice.
A simple and novel sample pretreatment method for determination of eight kinds of mycotoxin in juice samples has been developed using acid-assisted dispersive liquid-liquid microextraction coupled with high performance liquid chromatography-tandem mass spectrometry. The factors effecting extraction efficiency were investigated including the type and volume of extraction solvent,the volume of dispersive solvent and pH of the equilibrium system. Under the optimum extraction conditions including 60 μL of trichloroaniline as extraction solvent,1500 μL of hydrochloric acid solution as dispersive solvent and pH 5 as the acidity of equilibrium system,the method showed a good linearity for these mycotoxins within the concentration range from 1 to 500 μg/L with correlation coefficients higher than 0. 994. The detection limits were 0. 15-17. 71 ng/L,0.09-7.08 ng/L and 0. 40-14. 29 ng/L in fruit juice of mango,pineapple and dragon,respectively. The average recoveries of eight kinds of mycotoxins ranged from 75.6% to 110.0% at three spiked concentrations of 0.2 μg/L,1.0 μg/L and 10.0 μg/L,with the relative standard deviation of lower than 15.5%. The proposed method is simple,fast with less consumption of organic solvent,and has high sensitivity and repeatability,which is suitable for the detection of mycotoxins residues in fruit juice.
引文
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26 TENG Rui-Ju,WANG Huan,WANG Xue-Mei,SU Jia-Qiang,FENG Li-Juan,LU Xiao-Quan.Chinese J.Anal.Chem.,2017,45(2):275-281滕瑞菊,王欢,王雪梅,苏加强,冯丽娟.卢小泉.分析化学,2017,45(2):275-281
27 Rahmani M,Ghasemi E,Sasani M.Talanta,2017,165:27-32
28 Mohammadi A,Tavakoli R,Kamankesh M,Rashedi H,Attaran A,Delavar M.Anal.Chem.Acta,2013,804(23):104-110
29 Rodríguez-Carrasco Y,Ma1es J,Berrada H,Juan C.Toxins,2016,8(11):328
30 Lai X,Ruan C,Liu R,Liu C.Food Chem.,2014,16:317-322
31 Ruan C,Diao X,Li N,Zhang H,Pang Y,Liu C.Anal.Methods,2016,8(7):1586-1594
32 Hussein S,Jeffrey M B.Toxicology,2001,167(2):101-134
2 CHEN Li-Xing.Hebei Journal of Industrial Science and Technology,2006,23(2):124-126陈丽星.河北工业科技,2006,23(2):124-126
3 Amalaradjou M A R,Venkitanarayanan K.Mycotoxins Fruits Vegetables.Elsevier Academic Press,2008:225-247
4 FAN Zhi-Chen,HAN Zheng,GUO Wen-Bo,ZHAO Zhi-Hui.Chinese Journal of Chromatography,2017,35(6):627-633范志辰,韩铮,郭文博,赵志辉.色谱,2017,35(6):627-633
5 Scott P M,Van W W,Kennedy B,Anyeti D.J.Agric.Food Chem.,1972,20(6):1103-1109
6 WANG Yu-Jiao,NIE Ji-Yun,LI Zhi-Xia,YAN Zhen,CHENG Yang,ZHANG Xiao-Nan.Chinese J.Anal.Chem.,2017,45(10):1556-1563王玉娇,聂继云,李志霞,闫震,程杨,张晓男.分析化学,2017,45(10):1556-1563
7 Andersen B,Jrn S A,Frisvad J C.J.Agric.Food Chem.,2004,52(8):2421-2428
8 Barkai Golan R,Paster N.Mycotoxins in Fruits and Vegetables.Elsevier Academic Press,2008:147-159
9 Sweeney M J,Dobson A D.Int.Food Microbiol.,1998,43(3):141-158
10 WANG Meng,JIANG Nan,DAI Ying,FENG Xiao-Yuan.Food Safety and Quality Detection Technology,2016,7(2):459-467王蒙,姜楠,戴莹,冯晓元.食品安全质量检测学报,2016,7(2):459-467
11 Dos Santos I D,Pizzutti I R,Dias J V,Fontana M E Z,Brackmann A,Anese R O,Thewes F R,Marques L N,Cardoso C D.Food Chem.,2018,255:275-281
12 Yusefi J,Valaee M,Nazari F,Maleki J,Mottaghianpour E,Khosrokhavar R,Hosseini M J.Iran J.Pharm.Res.,2018,17(1):140-146
13 Bragulat M R,Abarca M L,Caba1es F J.Lett.Appl.Microbiol.,2010,47(4):286-289
14 Drusch S,Ragab W.J.Food Prot.,2003,66(8):1514-1527
15 GB 2761-2017,Limits of Mycotoxins in Food.National Food Safety Standards GB 2761-2017.食品中真菌毒素限量.食品安全国家标准
16 Commission Regulation(EC)No1881/2006,Setting Maximum Levels for Certain Contaminants in Foodstuffs
17 Tokusoglu O,Bozoglu F.Ital.J.Food Sci.,2010,22(3):284-291
18 WANG Heng-Ling,YU Li,LI Pei-Wu,LI Min,ZHANG Qi,ZHANG Wen.Chinese J.Anal.Chem.,2014,42(9):1338-1342王恒玲,喻理,李培武,李敏,张奇,张文.分析化学,2014,42(9):1338-1342
19 Arroyo-Manzanares N,De Ruyck K,Uka V,Gamiz-Gracia L,Garcia-Campana A M,De Saeger S,Diana D M J.Anal.Bioanal.Chem.,2018,65(23):1-15
20 Andrade P D,da Silva J L G,Caldas E D.J.Chromatogr.A,2013,1304:61-68
21 LIU Jia-Yang,ZHANG Yue-Hui,JIA Hong-Xin.Chinese Journal of Food Hygiene,2016,(6):763-768刘家阳,张月辉,贾宏新.中国食品卫生杂志,2016,(6):763-768
22 Radova Z,Hajslova J,Kralova J.Cereal Res.Commun.,2001,29(3-4):435-442
23 Rezaee M,Assadi Y,Hosseini M R M,Aghaee E,Ahmadi F,Berijani S.J.Chromatogr.A,2006,1116(1):1-9
24 XU Neng-Bin,FENG Jia-Yong,ZHU Li-Bo,QIAN Fei-Zhong,XU Li-Hong,CHEN Zhong-Quan,WANG Sheng-Le.Chinese J.Anal.Chem.,2016,44(1):117-123徐能斌,冯加永,朱丽波,钱飞中,徐立红,陈钟佺,汪晟乐.分析化学,2016,44(1):117-123
25 Socas-Rodríguez B,Hernndez-Borges J,Asensio-Ramos M,Herrera-Herrera A V,Palenzuela J A,Rodriguez-Delgado MA.Electrophoresis,2014,35(17):2479-2487
26 TENG Rui-Ju,WANG Huan,WANG Xue-Mei,SU Jia-Qiang,FENG Li-Juan,LU Xiao-Quan.Chinese J.Anal.Chem.,2017,45(2):275-281滕瑞菊,王欢,王雪梅,苏加强,冯丽娟.卢小泉.分析化学,2017,45(2):275-281
27 Rahmani M,Ghasemi E,Sasani M.Talanta,2017,165:27-32
28 Mohammadi A,Tavakoli R,Kamankesh M,Rashedi H,Attaran A,Delavar M.Anal.Chem.Acta,2013,804(23):104-110
29 Rodríguez-Carrasco Y,Ma1es J,Berrada H,Juan C.Toxins,2016,8(11):328
30 Lai X,Ruan C,Liu R,Liu C.Food Chem.,2014,16:317-322
31 Ruan C,Diao X,Li N,Zhang H,Pang Y,Liu C.Anal.Methods,2016,8(7):1586-1594
32 Hussein S,Jeffrey M B.Toxicology,2001,167(2):101-134