基于质谱断裂机理的乳制品中农药非定向筛查分析方法构建
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摘要
采用数据依赖型采集质谱技术,对585种农药标准物质的化合物分子离子质荷比、二级碎裂片段的质荷比与保留时间等进行研究,建立了农药残留标准数据库,并对8类100种农药进行片段断裂机理研究,得到不同类别农药的特征断裂片段。将特征断裂片段与农药残留标准数据库相结合,基于数据非依赖采集质谱技术,构建非定向筛查方法,方法检出限和检测容量分别为0.001～539μg/kg与0.001～899μg/kg,回收率与相对标准偏差分别为77%～113%和0.1%～8.3%。将所建立方法用于市售93个批次巴氏杀菌乳与超高温瞬时灭菌乳中农药的非定向分析,发现样品中含有前期未检出的嘧菌酯与草克乐,含量分别为2.3和6.1μg/kg。建立的非定向筛查分析方法可为快速筛查鉴定乳制品中农药提供有效的技术手段。
A method for non-target screening of pesticide residues in dairy products by ultra-high performance liquid chromatography-hybrid quadrupole-Orbitrap mass spectrometry(UHPLC-Q-Orbitrap MS) was developed. A database of pesticide residue standards was established for the experimental application of data-dependent acquisition mass spectrometry technology. Subsequently, the fragmentation mechanism of eight classes of 100 pesticides was studied, and the characteristic fracture fragments of different classes of pesticides were obtained. By combining pesticide fragmentation with the pesticide residue standard database, a non-directional screening method based on data-independent acquisition mass spectrometry was developed. Finally, the established method was applied to the non-directional analysis of pesticide residues in 93 batches of pasteurized milk and ultra-high temperature instant sterilized milk. As a result, pre-undetected azoxystrobin(2.3 μg/kg) and chlorthiamide(6.1 μg/kg) were detected in the samples, with the relative standard deviations of 2.3% and 1.2%. The high-resolution non-target screening analysis method established here can provide effective technical means for rapid screening and identification of pesticides in dairy products.
A method for non-target screening of pesticide residues in dairy products by ultra-high performance liquid chromatography-hybrid quadrupole-Orbitrap mass spectrometry(UHPLC-Q-Orbitrap MS) was developed. A database of pesticide residue standards was established for the experimental application of data-dependent acquisition mass spectrometry technology. Subsequently, the fragmentation mechanism of eight classes of 100 pesticides was studied, and the characteristic fracture fragments of different classes of pesticides were obtained. By combining pesticide fragmentation with the pesticide residue standard database, a non-directional screening method based on data-independent acquisition mass spectrometry was developed. Finally, the established method was applied to the non-directional analysis of pesticide residues in 93 batches of pasteurized milk and ultra-high temperature instant sterilized milk. As a result, pre-undetected azoxystrobin(2.3 μg/kg) and chlorthiamide(6.1 μg/kg) were detected in the samples, with the relative standard deviations of 2.3% and 1.2%. The high-resolution non-target screening analysis method established here can provide effective technical means for rapid screening and identification of pesticides in dairy products.
引文
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29 DONG Feng-Shou,LI Jing,LI Yuan-Bo,PAN Xing-Lu,XU Jun,LIU Xin-Gang,ZHENG Yong-Quan.Sci.China-VITAE,2016,46(5):613-618董丰收,李晶,李远播,潘兴鲁,徐军,刘新刚,郑永权.中国科学:生命科学,2016,46(5):613-618
30 WANG Xiao-Chun,LIU Qing-Long,YANG Yong-Liang.Chinese J.Anal.Chem.,2014,42(3):390-396王晓春,刘庆龙,杨永亮.分析化学,2014,42(3):390-396
31 Bahrami M,Laurienti P J,Quandt S A,Talton J,Pope C N,Summers P,Burdette J H,Chen H Y,Liu J,Howard T D,Arcury T A,Simpson S L.Neurotoxicology,2017,82:41-51
32 CHENG Yan-Hong,GE Jing,HU Gao-Jie,CAI Lei-Ming,CHEN Lie-Zhong,JIANG Jin-Hua.Asian J.Ecotoxicol.,2017,12(6):171-178程艳红,葛婧,胡高洁,蔡磊明,陈列忠,蒋金花.生态毒理学报,2017,12(6):171-178
2 Wu X L,Lu Y Q,Xu H X,Lv M Y,Hu D S,He Z D,Liu L Z,Wang Z M,Feng Y.Trends Food Sci.Tech.,2018,76:6-14
3 Han R W,Zheng N,Wang J Q,Zhen Y P,Xu X M,Li S L.Food Control,2013,34(1):35-39
4 SUN Xing-Quan,ZHAO Yu,YANG Chun-Guang,XU Jing,CAO Ji-Juan.Chinese Journal of Chromatography,2016,34(7):647-656孙兴权,赵禹,杨春光,徐静,曹际娟.色谱,2016,34(7):647-656
5 Knolhoff A M,Croley T R.J.Chromatogr.A,2016,1428:86-96
6 Sun Y P,Li L,Liao M,Su M,Wan C,Zhang L T,Zhang H L.J.Pharm.Biomed.Anal.,2018,154:216-226
7 Masia A,Suarez-Varela M M,Llopis-Gonzalez A,Pico Y.Anal.Chim.Acta,2016,936:40-61
8 Wang J,Chow W,Chang J,Wong J W.J.Agric.Food Chem.,2017,65(2):473-493
9 Jia W,Shi L,Chu X G,Chang J S,Chen Y,Zhang F.Food Chem.,2018,262:110-117
10 Wong J W,Wang J,Chow W,Carlson R,Jia Z W,Zhang K,Hayward D G,Chang J S.J.Agric.Food Chem.,2018,66:9573-9581
11 Zomer P,Mol H G.Food Addit.Contam.A,2015,32(10):1628-1636
12 Sharma A,Jha P,Reddy G V P.Sci.Total Environ.,2018,643:1522-1532
13 Marchis D,Ferro G L,Brizio P,Squadrone S,Abete M C.Food Control,2012,25(1):270-273
14 Muhammad N,Subhani Q,Wang F L,Lou C Y,Liu J W,Zhu Y.Food Chem.,2018,241:308-316
15 Jadhav M R,Pudale A,Raut P,Utture S,Shabeer T P A,Banerjee K.Food Chem.,2019,272:292-305
16 ZHANG Jing-Hua,YUAN Wen-Ting,GAO Zhan-Qi,SUN Cheng,YANG Shao-Gui,HE Huan,ZHANG Li-Min.Chinese J.Anal.Chem.,2018,46(10):1604-1609张晶华,原文婷,高占啟,孙成,杨绍贵,何欢,张利民.分析化学,2018,46(10):1604-1609
17 XUE Ping,DU Li-Jun,LIN Qin-Bao,CHEN Yong,SHI Hui-Juan.Journal of Instrumental Analysis,2010,29(9):948-952薛平,杜利君,林勤保,陈勇,史惠娟.分析测试学报,2010,29(9):948-952
18 Duan J,Cheng Z,Bi J W,Xu Y G.Food Chem.,2018,245:119-124
19 Laszlo N,Lanyi K,Laczay P.Food Chem.,2018,267:178-186
20 Grund B,Marvin L,Rochat B.J.Pharm.Biomed.Anal.,2016,124:48-56
21 Yang P,Chang J S,Wong J W,Zhang K,Krynitsky A J,Bromirski M,Wang J.J.Agric.Food Chem.,2015,63:5169-5177
22 Wang J,Chow W,Chang J,Wong J W.J.Agric.Food Chem.,2017,65(2):473-493
23 Kumar K,Siva B,Rao R N,Babua K S.J.Pharmaceut.Biomed.,2018,152:224-233
24 SHAO Yang,YANG Guo-Sheng,HAN Shen,MA Ling-Ling,LUO Min,LIU Wei-Hua,XU Dian-Dou.Chinese J.Anal.Chem.,2016,44(5):698-706邵阳,杨国胜,韩深,马玲玲,罗敏,刘韦华,徐殿斗.分析化学,2016,44(5):698-706
25 WANG Yi,ZHANG Pin,WU Sheng-Xiu,SUN Yuan-Yuan,ZHAO Tong,LIU Shi-Xi.Chem.J.Chinses University,2018,39(3):435-446王毅,张苹,吴生秀,孙媛媛,赵彤,刘世熙.高等学校化学学报,2018,39(3):435-446
26 Samsidar A,Siddiquee S,Shaarani S M.Trends Food Sci.Tech.,2017,71:188-201
27 LUO Hui-Tai,HUANG Xiao-Lan,WU Hui-Qin,ZHANG Li,GUO Yin-Long,ZHU Zhi-Xin,HUANG Fang,LIN XiaoShan.Chinese J.Anal.Chem.,2014,42(11):1561-1567罗辉泰,黄晓兰,吴惠勤,张立,郭寅龙,朱志鑫,黄芳,林晓珊.分析化学,2014,42(11):1561-1567
28 Tang W X,Wang D,Wang J Q,Wu Z W,Li L Y,Huang M L,Xu S H,Yan D Y.Chemosphere,2018,192:990-1007
29 DONG Feng-Shou,LI Jing,LI Yuan-Bo,PAN Xing-Lu,XU Jun,LIU Xin-Gang,ZHENG Yong-Quan.Sci.China-VITAE,2016,46(5):613-618董丰收,李晶,李远播,潘兴鲁,徐军,刘新刚,郑永权.中国科学:生命科学,2016,46(5):613-618
30 WANG Xiao-Chun,LIU Qing-Long,YANG Yong-Liang.Chinese J.Anal.Chem.,2014,42(3):390-396王晓春,刘庆龙,杨永亮.分析化学,2014,42(3):390-396
31 Bahrami M,Laurienti P J,Quandt S A,Talton J,Pope C N,Summers P,Burdette J H,Chen H Y,Liu J,Howard T D,Arcury T A,Simpson S L.Neurotoxicology,2017,82:41-51
32 CHENG Yan-Hong,GE Jing,HU Gao-Jie,CAI Lei-Ming,CHEN Lie-Zhong,JIANG Jin-Hua.Asian J.Ecotoxicol.,2017,12(6):171-178程艳红,葛婧,胡高洁,蔡磊明,陈列忠,蒋金花.生态毒理学报,2017,12(6):171-178
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