Determination of Multi-pesticide Residues in Tea Based on the Combination of CS/GO/DM SPE Column and UPLC-MS/MS

HU Gaohua; CAO Jianrong; YANG-LEI Wenxuan; WANG Chen; ZHOU Sujuan; LIU Xin; LU Chengyin; CHEN Hongping; MA Guicen

doi:10.13305/j.cnki.jts.2022.02.004

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Journal of Tea Science ›› 2022, Vol. 42 ›› Issue (2) : 249-262. DOI: 10.13305/j.cnki.jts.2022.02.004

Research Paper

Determination of Multi-pesticide Residues in Tea Based on the Combination of CS/GO/DM SPE Column and UPLC-MS/MS

HU Gaohua^1,2,3,4, CAO Jianrong^1,3,4, YANG-LEI Wenxuan^1,2,3,4, WANG Chen^1,3,4, ZHOU Sujuan^1,3,4, LIU Xin^1,3,4, LU Chengyin^1,3,4, CHEN Hongping^1,3,4, MA Guicen^1,3,4,*

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Abstract

In this study, the synthesized chitosan/graphene oxide/diatomite (CS/GO/DM) solid phase extraction (SPE) column cartridge was used for the purification of tea matrix. A method for determination of 46 kinds of pesticide residues in tea by using ultra-high performance liquid chromatography-tandem mass spectrometry (UPLC-MS/MS) was established. The tea samples were extracted by acetonitrile, purified by CS/GO/DM SPE column, washed by acetonitrile. Then, the target compounds of 46 pesticide residues were analyzed by UPLC-MS/MS. The results show that CS/GO/DM SPE column could efficiently remove tea interference substances, which could greatly reduce the matrix effect of pesticides in green tea, black tea and oolong tea by 4.7%-66.5%, 3.2%-35.5% and 4.4%-42.8%, respectively. The recoveries of 46 kinds of pesticides ranged from 61.5% to 118% at three spiked levels, with good linearity. The correlation coefficients (R²) were all higher than 0.98. The developed method has the great advantages of operation simplicity, time saving, and high cleanup ability with only one kind towards different types of tea, no need for using matrix standard solution and a low amount of adsorbent.

Key words

CS/GO/DM / matrix purification / pesticide residues / tea / UPLC-MS/MS

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HU Gaohua, CAO Jianrong, YANG-LEI Wenxuan, WANG Chen, ZHOU Sujuan, LIU Xin, LU Chengyin, CHEN Hongping, MA Guicen. Determination of Multi-pesticide Residues in Tea Based on the Combination of CS/GO/DM SPE Column and UPLC-MS/MS[J]. Journal of Tea Science. 2022, 42(2): 249-262 https://doi.org/10.13305/j.cnki.jts.2022.02.004

References

[1] 刘新, 陈红平, 王国庆. 中国茶叶质量安全40年[J]. 中国茶叶, 2019, 41(12): 1-9.
Liu X, Chen H P, Wang G Q.Quality and safety of Chinese tea for 40 years[J]. China tea, 2019, 41(12): 1-9.
[2] Li C, Zhu H, Li C, et al.The present situation of pesticide residues in China and their removal and transformation during food processing[J]. Food Chemistry, 2021, 354(2): 129552. doi: 10.1016/j.foodchem.2021.129552.
[3] Sun R, Yang W Q, Li Y X, et al.Multi-residue analytical methods for pesticides in teas: a review[J]. European Food Research and Technology, 2021, 247(8): 1839-1858.
[4] Soler C, Manes J, Pico Y.The role of the liquid chromatography-mass spectrometry in pesticide residue determination in food[J]. Critical Reviews in Analytical Chemistry, 2008, 38(2): 93-117
[5] Kruve A, Kuennapas A, Herodes K, et al.Matrix effects in pesticide multi-residue analysis by liquid chromatography-mass spectrometry[J]. Journal of Chromatography A, 2008, 1187(1/2): 58-66.
[6] Besil N, Cesio V, Heinzen H, et al.Matrix effects and interferences of different citrus fruit coextractives in pesticide residue analysis using ultrahigh-performance liquid chromatography-high-resolution mass spectrometry[J]. Journal of Agricultural and Food Chemistry, 2017, 65(23): 4819-4829.
[7] Oellig C, Schwack W.Planar solid phase extraction clean-up for pesticide residue analysis in tea by liquid chromatography-mass spectrometry[J]. Journal of Chromatography A, 2012, 1260: 42-53.
[8] Pascoe R, Foley J P, Gusev A I.Reduction in matrix-related signal suppression effects in electrospray ionization mass spectrometry using on-line two-dimensional liquid chromatography[J]. Analytical Chemistry, 2001, 73(24): 6014-6023.
[9] Kmellar B, Pareja L, Ferrer C, et al.Study of the effects of operational parameters on multiresidue pesticide analysis by LC-MS/MS[J]. Talanta, 2011, 84(2): 262-273.
[10] Guironnet A, Wiest L, Vulliet E.Improvement of the QuEChERS extraction step by matrix-dispersion effect and application on beta-lactams analysis in wastewater sludge by LC-MS/MS[J]. Talanta, 2022, 237: 122923. doi: 10.1016/j.talanta.2021.122923.
[11] Guo Y, Zhang J, Xu J, et al.An integrated strategy for purification by combining solid-phase extraction with dispersive-solid-phase extraction for detecting 22 pesticides and metabolite residues in fish[J]. Journal of Agricultural and Food Chemistry, 2021, 69(25): 7199-7208.
[12] Anastassiades M, Lehotay S J, Stajnbaher D, et al.Fast and easy multiresidue method employing acetonitrile extraction/partitioning and "dispersive solid-phase extraction" for the determination of pesticide residues in produce[J]. Journal of AOAC International, 2003, 86(2): 412-431.
[13] Ferrer C, Lozano A, Agueera A, et al.Overcoming matrix effects using the dilution approach in multiresidue methods for fruits and vegetables[J]. Journal of Chromatography A, 2011, 1218(42): 7634-7639.
[14] Jiao W, Xiao Y, Qian X, et al.Optimized combination of dilution and refined QuEChERS to overcome matrix effects of six types of tea for determination eight neonicotinoid insecticides by ultra performance liquid chromatography-electrospray tandem mass spectrometry[J]. Food Chemistry, 2016, 210: 26-34.
[15] Ma G C, Cao J R, Hu G H, et al.Porous chitosan/partially reduced graphene oxide/diatomite composite as an efficient adsorbent for quantitative colorimetric detection of pesticides in a complex matrix[J]. Analyst (London), 2021, 146(14): 4576-4584.
[16] Hummers W S, Offeman R E.Preparation of graphitic oxide[J]. Journal of the American Chemical Society, 1958, 80: 1339. doi: 10.1021/ja01539a017.
[17] Huang Y S, Shi T, Luo X, et al.Determination of multi-pesticide residues in green tea with a modified QuEChERS protocol coupled to UPLC-MS/MS[J]. Food Chemistry, 2019, 275: 255-264.
[18] Chen G Q, Cao P Y, Liu R J.A multi-residue method for fast determination of pesticides in tea by ultra performance liquid chromatography-electrospray tandem mass spectrometry combined with modified QuEChERS sample preparation procedure[J]. Food Chemistry, 2011, 125(4): 1406-1411.
[19] Huang Z Q, Zhang Y, Wang L B, et al.Simultaneous determination of 103 pesticide residues in tea samples by LC-MS/MS[J]. Journal of Separation Science, 2009, 32: 1294-1301.
[20] Xie W, Han C, Qian Y, et al.Determination of neonicotinoid pesticides residues in agricultural samples by solid-phase extraction combined with liquid chromatography-tandem mass spectrometry[J]. Journal of Chromatography A, 2011, 1218(28): 4426-4433.
[21] 国家卫生健康委员会, 农业农村部和国家市场监督管理总局. 食品安全国家标准食品中农药最大残留限量: GB 2763—2019[S]. 北京: 中国标准出版社, 2019.
The National Health Commission, the Ministry of Agriculture and Rural Affairs and the State Administration for Market Regulation. National Food Safety Standard Maximum residue limits of pesticides in food: GB 2763—2019 [S]. Beijing: Standards Press of China, 2019.