Development and Validation of a Liquid Chromatography–Tandem Mass Spectrometry Method for Multiresidue Determination of 25 Herbicides in Soil and Tobacco

  • Ya Chen
  • Yurong Yu
  • Xiangwu Liu
  • Ya Yang
  • Ping LuEmail author
  • Deyu HuEmail author


In the cultivation of tobacco, crop rotation patterns, such as tobacco/rice or tobacco/corn, are widely used. However, the use of herbicides in the rice or corn phase can lead to their being taken in during the tobacco phase by inner conduction action. In the present study, to monitor the use of herbicides in tobacco, a sensitive and simple analytical method coupled with liquid chromatography-tandem mass spectrometry (LC–MS/MS) has been established for determination of 25 herbicides in soil as well as fresh and flue-cured tobacco leaf. The herbicides analyzed include six aryloxy phenoxy propionate herbicides (APPs) and 19 sulfonylureas herbicides (SUs). The samples were extracted using acetonitrile and purified using C18 sorbent before analysis. Optimum separation of the analytes was achieved using an Agilent Eclipse XDB-C18 column at 40 °C and gradient elution with acetonitrile and 0.1% aqueous formic acid as the mobile phase at a flow rate of 0.8 mL min−1. The limits of quantification and detection are in the ranges 0.08–1.00 mg kg−1 and 0.024–0.30 mg kg−1, respectively, and matrix effects in the range − 70 to 50% were achieved. The recovery rates obtained from spiked soil and tobacco leaf samples ranged from 72.32 to 116.83% with intra-day and inter-day relative standard deviations of 0.44–11.55%. In addition, the method developed was applied to the determination of herbicides residues in actual soil and tobacco samples, revealing that the proposed method can detect trace amounts of APPs and SUs in soil as well as in fresh and flue-cured tobacco leaf.

Graphic Abstract


Liquid chromatography–tandem mass spectrometry (LC–MS/MS) Aryloxy phenoxy propionate herbicide Sulfonylurea herbicide Tobacco Soil 


Author Contributions

The formulation of overarching research goals and aims were performed by [DH] and [PL]. Development of methodology was conducted by [YC] and [YY]. Material preparation, provision data collection and analysis were performed by [YC], [YY], [XL] and [YY]. The first draft of the manuscript was written by [YC] and all authors commented on previous versions of the manuscript. All authors read and approved the final manuscript.


This study was funded by the National Key Research and Development Program of China (Grant number 2016YFD0201305) and the Science and Technology Programs of Guizhou Province (Grant number [2019]2347).

Compliance with Ethical Standards

Conflict of Interest

All authors declare that they have no conflict of interest.

Ethical Approval

This article does not contain any studies with human participants or animals performed by the authors.

Supplementary material

10337_2019_3834_MOESM1_ESM.pdf (836 kb)
Supplementary material 1 (PDF 835 kb)


  1. 1.
    Wang XG, Xu GJ, Wang FL, Sun HQ, Li YQ (2012) Bull Environ Contam Toxicol 89:877–881PubMedCrossRefGoogle Scholar
  2. 2.
    Wang F, Yang GQ, Xu J, Yu WW, Shi LH, Zeng S, Chen LZ, Hu DY, Zhang KK (2018) Biomed Chromatogr 32:e4148CrossRefGoogle Scholar
  3. 3.
    FAO (Food and Agriculture Organization of the United Nations) Crop Statistics (2017). Accessed 05 March 2019
  4. 4.
    Farajzadeh MA, Mohebbi A, Feriduni B (2016) Anal Chim Acta 920:1–9PubMedCrossRefGoogle Scholar
  5. 5.
    Ni YX, Yang H, Zhang HT, He Q, Huang SQ, Qin ML, Chai SS, Cao HH, Ma YN (2018) J Chromatogr A 1537:27–34PubMedCrossRefGoogle Scholar
  6. 6.
    Lucini L, Molinari GP (2011) Qual Assur Saf Crops Foods 3:63–68CrossRefGoogle Scholar
  7. 7.
    Gronwald JW (2015) Biochem Soc Trans 22:616–621CrossRefGoogle Scholar
  8. 8.
    Hu JY, Deng ZB, Liu C, Zheng ZX (2010) Chromatographia 72:701–706CrossRefGoogle Scholar
  9. 9.
    Farajzadeh MA, Yadeghari A, Khoshmaram L (2017) Microchem J 131:182–191CrossRefGoogle Scholar
  10. 10.
    Seccia S, Albrizio S, Fidente P, Montesano D (2011) J Chromatogr A 1218:1253–1259PubMedCrossRefGoogle Scholar
  11. 11.
    Seebunrueng K, Santaladchaiyakit Y, Srijaranai S (2013) Anal Methods 5:6009–6016CrossRefGoogle Scholar
  12. 12.
    Gure A, Lara FJ, Moreno-González D, Megersa N, Del Olmo-Iruela M, García-Campaña AM (2014) Talanta 127:51–58PubMedCrossRefGoogle Scholar
  13. 13.
    Ghobadi M, Yamini Y, Ebrahimpour B (2015) Ecotoxicol Environ Saf 112:68–73PubMedCrossRefGoogle Scholar
  14. 14.
    Rejczak T, Tuzimski T (2016) J Chromatogr A 147:56–65CrossRefGoogle Scholar
  15. 15.
    Mehdizadeh M, Alebrahim MT, Roushani M (2017) Bull Environ Contam Toxicol 99:93–99PubMedCrossRefGoogle Scholar
  16. 16.
    Fenoll J, Hellín P, Sabater P, Flores P, Navarro S (2012) Talanta 101:273–282PubMedCrossRefGoogle Scholar
  17. 17.
    Lee YJ, Rahman MM, Abd El-Aty AM, Choi JH, Chun HS, Kim SW, Abdel-Aty AM, Shin HC, Shim JH (2016) Food Chem 210:442–450PubMedCrossRefGoogle Scholar
  18. 18.
    Kaczyński P, Łozowicka B (2017) Food Anal Methods 10:147–160CrossRefGoogle Scholar
  19. 19.
    Chen XX, Yu S, Han LJ, Sun SJ, Zhi YA, Li WM (2011) Bull Environ Contam Toxicol 87:50–53PubMedCrossRefPubMedCentralGoogle Scholar
  20. 20.
    Wu YB, Liu XG, Dong FS, Xu J, Zheng YQ (2012) Bull Environ Contam Toxicol 89:1264–1267PubMedCrossRefGoogle Scholar
  21. 21.
    Yan CM, Zhang BB, Liu WY, Feng F, Zhao YG, Du H (2011) J Chromatogr B 879:3484–3489CrossRefGoogle Scholar
  22. 22.
    Sheng JC, Xu ZX, Cai JB, Shao XG (2006) Anal Sci 22:241–244CrossRefGoogle Scholar
  23. 23.
    Li Y, Zhu J, Ren L, Li YX, Zou XL (2016) J Braz Chem Soc 27:1792–1799Google Scholar
  24. 24.
    Liu HX, Ding CH, Zhang SS, Liu HM, Liao XC, Qu LB, Zhao YF, Wu YJ (2004) J Agric Food Chem 52:6912–6915PubMedCrossRefGoogle Scholar
  25. 25.
    Luo YB, Li X, Jiang XY, Cai BD, Zhu FP, Zhang HF, Chen ZG, Pang YQ, Feng YQ (2015) J Chromatogr A 1406:1–9PubMedCrossRefGoogle Scholar
  26. 26.
    Anastassiade M, Lehotay SJ (2003) J AOAC Int 86:412–431Google Scholar
  27. 27.
    Fernanda RBK, Márcia CB, Isabel CSFJ (2017) J Chromatogr A 1482:11–22CrossRefGoogle Scholar
  28. 28.
    Agricultural Industry Standards of the People’s Republic of China (NY/T 1121) Guidance document on soil testing. Accessed 12 March 2019
  29. 29.
    Liu GS, Liu JL (2010) Practical guide to leaf tobacco production techniques in China. China National Leaf Tobacco Corporation, BeijingGoogle Scholar
  30. 30.
    Zhang QT, Yang Y, Liu XW, Chen Y, Hu DY, Lu P (2019) Anal Lett 52:948–961sCrossRefGoogle Scholar
  31. 31.
    Han YT, Zou N, Song L, Li YJ, Qin YH, Liu SW, Li XS, Pan CP (2015) J Chromatogr B 1005:56–64CrossRefGoogle Scholar
  32. 32.
    de Gimenes Souza C, de Torres Araújo M, Cavalcante dos Santos R, de França Andrade D, da Vasconcello Silva B, Antonio d’Avila L (2018) Energy Fuels 32:11547–11554CrossRefGoogle Scholar
  33. 33.
    Kim NS, Kim KY, Yoo GJ, Lee JH, Park HN, Park SK, Baek SY (2018) Food Addit Contam Part A 35:387–394CrossRefGoogle Scholar
  34. 34.
    Arrebola FJ, Cortes Aguado S, Sánchez-Morito N, Garrido Frenich A, Martínez Vidal JL (2004) Anal Lett 37:99–117CrossRefGoogle Scholar
  35. 35.
    Rutkowska E, Łozowicka B, Kaczyński P (2019) Food Chem 279:20–29PubMedCrossRefGoogle Scholar
  36. 36.
    Yang F, Bian ZY, Chen XS, Liu SS, Liu Y, Tang GL (2014) J Chromatogr Sci 52:788–792PubMedCrossRefGoogle Scholar
  37. 37.
    Zhou X, Cao SR, Li XL, Tang BB, Ding XW, Xi CX, Hu JT, Chen ZQ (2015) J Chromatogr B 989:21–26CrossRefGoogle Scholar
  38. 38.
    Zhou X, Cao SR, Li XL, Xi CX, Ding XW, Xu F, Hu JT, Chen ZQ (2016) J Chromatogr Sci 54:858–863PubMedPubMedCentralCrossRefGoogle Scholar
  39. 39.
    Dorival-García N, Junza A, Zafra-Gómez A, Barrónb D, Navalóna A (2016) Food Control 60:382–393CrossRefGoogle Scholar
  40. 40.
    Qin YH, Zhao PY, Fan SF, Han YT, Li YJ, Zou N, Song SY, Zhang Y, Li FB, Li XS, Pan CP (2015) J Chromatogr A 1385:1–11PubMedCrossRefPubMedCentralGoogle Scholar
  41. 41.
    Tian CY, Xu J, Dong FS, Liu XG, Wu XH, Zhao HH, Ju C, Wei DM, Zheng YQ (2016) J Agric Food Chem 64:2641–2646PubMedCrossRefPubMedCentralGoogle Scholar
  42. 42.
    Zhao HH, Xu J, Dong FS, Liu XG, Wu YB, Zhang JG, Zheng YQ (2014) Anal Methods 6:4336–4342CrossRefGoogle Scholar
  43. 43.
    Tripathy V, Sharma KK, Yadav R, Devi S, Tayade A, Sharma K, Pandey P, Singh G, Patel AN, Gautam R, Gupta R, Kalra S, Shukla P, Walia S, Shakil NA (2019) J Environ Sci Health, Part B 54:394–406CrossRefGoogle Scholar
  44. 44.
    Colazzo M, Pareja L, Cesio MV, Heinzen H (2018) Int J Environ Anal Chem 98:1292–1308CrossRefGoogle Scholar
  45. 45.
    Cao YL, Tang H, Chen DZ, Li L (2015) J Chromatogr B 998–999:72–79CrossRefGoogle Scholar
  46. 46.
    National Food Administration (2018) Guidance document on analytical quality control and method validation procedures for pesticide residues analysis in food and feed (SANTE/11813/2017)., 2017. Accessed 15 March 2019

Copyright information

© Springer-Verlag GmbH Germany, part of Springer Nature 2019

Authors and Affiliations

  1. 1.Key Laboratory of Green Pesticide and Agricultural Bioengineering, Ministry of Education, Center for Research and Development of Fine ChemicalsGuizhou UniversityGuiyangPeople’s Republic of China

Personalised recommendations