基于磁纳米材料的土壤中多农药残留高通量分析技术研究
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摘要
建立了土壤中43种农药及代谢物残留的高通量分析方法。土壤样品经乙腈超声萃取后,采用分散固相萃取法进一步对萃取液进行净化。选择修饰N-丙基乙二胺(PSA)的Fe_3O_4磁纳米材料和C_(18)为分散净化吸附剂,采用超高效液相色谱-串联质谱(UPLC-MS/MS)分析。优化实验结果表明,超声萃取时间为10 min、净化吸附剂Fe_3O_4-PSA用量为40 mg、C_(18)用量为30 mg时,农药的回收率最佳。除3-羟基克百威和水胺硫磷(5～250μg/L)外,各农药在2～250μg/L范围内呈良好线性关系,相关系数(R)均大于0.9700,检出限为0.1～1.0μg/L。在10、100和200μg/kg的添加浓度下,目标分析物在土壤中的回收率在74.1%～120.0%之间,相对标准偏差≤18.1%。本方法前处理过程简单,灵敏度高,净化效果好,适用于土壤中多农药残留分析。
A simple and rapid sample pretreatment method was developed based on magnetic nanoparticles for multi-pesticides residue analysis in soil samples. The target analytes were extracted by acetonitrile under the assistance of ultra-sonication,followed by the purification of dispersive solid phase extraction. The magnetite(Fe_3O_4) nanoparticles modified with 3- (N,N-diethylamino) propyltrimethoxysilane (Fe_3O_4-PSA) and commercial C_(18) were selected as the cleanup adsorbents to remove the matrix interferences. The target analytes were further analyzed by ultra-high performance liquid chromatography-tandem mass spectrometry (UHPLCMS/MS). The factors influencing the recoveries of analytes,such as extraction time,amount of Fe_3O_4-PSA and C_(18),were optimized. The optimal extraction time was 10 min,and the amount of Fe_3O_4-PSA and C_(18) were 40 mg and 30 mg,respectively. The method showed good linearity in the concentration range from 2 μg/L to 250 μg/L except for 3-hydroxy-carbofuran and isocarbophos (5 μg/L to 250 μg/L). The limits of detection(LODs) ranged from 0.1 μg/L to 1.0 μg/L. The recoveries ranged from 74.1% to 120.0% at three spiked concentration levels with relative standard deviations of lower than 18.1%. The proposed method was rapid,simple,low-cost and effective for detection of trace multi-pesticides residue in soil.
A simple and rapid sample pretreatment method was developed based on magnetic nanoparticles for multi-pesticides residue analysis in soil samples. The target analytes were extracted by acetonitrile under the assistance of ultra-sonication,followed by the purification of dispersive solid phase extraction. The magnetite(Fe_3O_4) nanoparticles modified with 3- (N,N-diethylamino) propyltrimethoxysilane (Fe_3O_4-PSA) and commercial C_(18) were selected as the cleanup adsorbents to remove the matrix interferences. The target analytes were further analyzed by ultra-high performance liquid chromatography-tandem mass spectrometry (UHPLCMS/MS). The factors influencing the recoveries of analytes,such as extraction time,amount of Fe_3O_4-PSA and C_(18),were optimized. The optimal extraction time was 10 min,and the amount of Fe_3O_4-PSA and C_(18) were 40 mg and 30 mg,respectively. The method showed good linearity in the concentration range from 2 μg/L to 250 μg/L except for 3-hydroxy-carbofuran and isocarbophos (5 μg/L to 250 μg/L). The limits of detection(LODs) ranged from 0.1 μg/L to 1.0 μg/L. The recoveries ranged from 74.1% to 120.0% at three spiked concentration levels with relative standard deviations of lower than 18.1%. The proposed method was rapid,simple,low-cost and effective for detection of trace multi-pesticides residue in soil.
引文
1 Jana V,Martina H,Petra K,Jakub H.Chemosphere,2018,216:479-487
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9 Pang N,Wang T,Hu J.Food Chem.,2016,190:793-800
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13 Peng X T,Jiang L,Gong Y,Hu X Z,Peng L J,Feng Y Q.Talanta,2015,132:118-125
14 Qi P P,Wang Z W,Yang G L,Shang C Q,Xu H,Wang X Y,Zhang H,Wang Q,Wang X Q.Microchim.Acta,2015,182:2521-2528
15 Wang P C,Lee R J,Chen C Y,Chou C C,Lee M R.Anal.Chim Acta,2012,752:78-86
16 Virginia M,Eulogio J M,Mohammed Z,Angel R.J.Supercrit.Fluid.,2018,137:66-73
17 LIU Hui,ZHANG Yan.Food Safety and Quality Detection Technology.,2015,6(4):1307-1313刘辉,张燕.食品安全质量检测学报,2015,6(4):1307-1313
18 SANTE/11945/2015,Guidance Document on Analytical Quality Control and Method Validation Procedures for Pesticides Residues Analysis in Food and Feed.European Commission
19 Liu Z Z,Qi P P,Wang X Y,Wang Z W,Xu X H,Chen W X,Wu L Y,Zhang H,Wang Q,Wang X Q.Food Chem.,2017,230:423-431
20 Zhang H,Wang X Q,Zhuang S L,Jin N,Wang X Q,Qian M R,Xu H,Qi P P,Wang Q,Wang M H.Food Chem.,2012,60:10188-10195
2 Natalia N,Marek T,Marketa S,Jana V,Zdenek S,Jakub H,Lucie B.Sci.Total Envirron.,2019,646:1056-1062
3 Li Z J.Environ.Int.,2018,121:620-634
4 Marta P B.,Isabel G,Natalia C,Pilar V,Hellin P,Flores P,Fenoll J.J.Chromatogr.A,2015,1394:1-8
5 LIU Hong-Mei,LI Xiao-Peng,LI Wen-Ying,HAN Hai-Tao.Guangdong Agricultural Sciences,2012,39(11):188-190刘红梅,黎小鹏,李文英,韩海涛.广东农业科学,2012,39(11):188-190
6 WU Yan,NIU Yan,CHEN Xiang,YANG Jing.Agrochemicals,2017,56(07):515-517吴燕,牛艳,陈翔,杨静.农药,2017,56(07):515-517
7 Naeeni M H,Yamini Y,Rezaee M,Seidi S.J.Sep.Sci.,2012,35:2469-2475
8 Zhao P F,Wang Z K,Li K J,Guo X J,Zhao L S.J.Chromatogr.A,2018,1568:8-21
9 Pang N,Wang T,Hu J.Food Chem.,2016,190:793-800
10 CHEN Lin-Ji,ZHU Chao-Le,CAO Xiao-Ji,ZHOU Ting,YE Xue-Min,MO Wei-Min.Chinese J.Anal.Chem.,2017,45(5):762-769陈林吉,朱晁乐,曹小吉,周婷,叶学敏,莫卫民.分析化学,2017,45(5):762-769
11 WANG Zhi,WANG Chun.Chinese Journal of Chromatography,2012,30(10):977-979王志,王春.色谱,2012,30(10):977-979
12 Gao Q,Luo D,Ding J,Feng Y Q.J.Chromatogr.A,2010,1217:5602-5609
13 Peng X T,Jiang L,Gong Y,Hu X Z,Peng L J,Feng Y Q.Talanta,2015,132:118-125
14 Qi P P,Wang Z W,Yang G L,Shang C Q,Xu H,Wang X Y,Zhang H,Wang Q,Wang X Q.Microchim.Acta,2015,182:2521-2528
15 Wang P C,Lee R J,Chen C Y,Chou C C,Lee M R.Anal.Chim Acta,2012,752:78-86
16 Virginia M,Eulogio J M,Mohammed Z,Angel R.J.Supercrit.Fluid.,2018,137:66-73
17 LIU Hui,ZHANG Yan.Food Safety and Quality Detection Technology.,2015,6(4):1307-1313刘辉,张燕.食品安全质量检测学报,2015,6(4):1307-1313
18 SANTE/11945/2015,Guidance Document on Analytical Quality Control and Method Validation Procedures for Pesticides Residues Analysis in Food and Feed.European Commission
19 Liu Z Z,Qi P P,Wang X Y,Wang Z W,Xu X H,Chen W X,Wu L Y,Zhang H,Wang Q,Wang X Q.Food Chem.,2017,230:423-431
20 Zhang H,Wang X Q,Zhuang S L,Jin N,Wang X Q,Qian M R,Xu H,Qi P P,Wang Q,Wang M H.Food Chem.,2012,60:10188-10195