Skip to main content
SpringerLink
Log in

Utilizing ion mobility spectrometry-mass spectrometry for the characterization and detection of persistent organic pollutants and their metabolites

  • Research Paper
  • Published:
Analytical and Bioanalytical Chemistry Aims and scope Submit manuscript

Abstract

Persistent organic pollutants (POPs) are xenobiotic chemicals of global concern due to their long-range transport capabilities, persistence, ability to bioaccumulate, and potential to have negative effects on human health and the environment. Identifying POPs in both the environment and human body is therefore essential for assessing potential health risks, but their diverse range of chemical classes challenge analytical techniques. Currently, platforms coupling chromatography approaches with mass spectrometry (MS) are the most common analytical methods employed to evaluate both parent POPs and their respective metabolites and/or degradants in samples ranging from d rinking water to biofluids. Unfortunately, different types of analyses are commonly needed to assess both the parent and metabolite/degradant POPs from the various chemical classes. The multiple time-consuming analyses necessary thus present a number of technical and logistical challenges when rapid evaluations are needed and sample volumes are limited. To address these challenges, we characterized 64 compounds including parent per- and polyfluoroalkyl substances (PFAS), pesticides, polychlorinated biphenyls (PCBs), industrial chemicals, and pharmaceuticals and personal care products (PPCPs), in addition to their metabolites and/or degradants, using ion mobility spectrometry coupled with MS (IMS-MS) as a potential rapid screening technique. Different ionization sources including electrospray ionization (ESI) and atmospheric pressure photoionization (APPI) were employed to determine optimal ionization for each chemical. Collectively, this study advances the field of exposure assessment by structurally characterizing the 64 important environmental pollutants, assessing their best ionization sources, and evaluating their rapid screening potential with IMS-MS.

This is a preview of subscription content, log in via an institution to check access.

Access this article

Log in via an institution

Price excludes VAT (USA)
Tax calculation will be finalised during checkout.

Instant access to the full article PDF.

Institutional subscriptions

Fig. 1
Fig. 2
Fig. 3
Fig. 4
Fig. 5
Fig. 6
Fig. 7

Similar content being viewed by others

References

  1. Tang HP. Recent development in analysis of persistent organic pollutants under the Stockholm Convention. Trends Anal Chem. 2013;45.

  2. Wang T, Wang Y, Liao C, Cai Y, Jiang G. Perspectives on the inclusion of perfluorooctane sulfonate into the Stockholm Convention on persistent organic pollutants. Environ Sci Technol. 2009;43(14):5171–5.

    Article  PubMed  CAS  Google Scholar 

  3. Richardson SD, Kimura SY. Water analysis: emerging contaminants and current issues. Anal Chem. 2020;92(1):473–505.

    Article  PubMed  CAS  Google Scholar 

  4. Richmond EK, Grace MR, Kelly JJ, Reisinger AJ, Rosi EJ, Walters DM. Pharmaceuticals and personal care products (PPCPs) are ecological disrupting compounds (EcoDC). Elementa-Sci Anthrop 2017;5.

  5. Omiecinski CJ, Vanden Heuvel JP, Perdew GH, Peters JM. Xenobiotic metabolism, disposition, and regulation by receptors: from biochemical phenomenon to predictors of major toxicities. Toxicol Sci. 2011;120(Suppl 1):S49–75.

    Article  PubMed  CAS  Google Scholar 

  6. Zacharia JT. Degradation pathways of persistent organic pollutants (POPs) in the environment. In: Donyinah SK, editor. Persistent organic pollutants. London, UK: IntechOpen; 2019.

    Google Scholar 

  7. Vermeulen R, Schymanski EL, Barabasi AL, Miller GW. The exposome and health: where chemistry meets biology. Science. 2020;367(6476):392–6.

    Article  PubMed  PubMed Central  CAS  Google Scholar 

  8. Liu K, Lee C, Singer G, Woodworth M, Ziegler TR, Kraft C, et al. Large-scale, enzyme-based xenobiotic identification for exposomics. Nature Communications. 2021.

  9. Aly NA, Casillas G, Luo YS, McDonald TJ, Wade TL, Zhu R, et al. Environmental impacts of Hurricane Florence flooding in eastern North Carolina: temporal analysis of contaminant distribution and potential human health risks. J Expo Sci Environ Epidemiol 2021; 31(5)810–822.

  10. Dodds JN, Alexander NLM, Kirkwood KI, Foster MR, Hopkins ZR, Knappe DRU, et al. From pesticides to per- and polyfluoroalkyl substances: an evaluation of recent targeted and untargeted mass spectrometry methods for xenobiotics. Anal Chem. 2021;93(1):641–56.

    Article  PubMed  CAS  Google Scholar 

  11. Zhang X, Romm M, Zheng X, Zink EM, Kim YM, Burnum-Johnson KE, et al. SPE-IMS-MS: an automated platform for sub-sixty second surveillance of endogenous metabolites and xenobiotics in biofluids. Clin Mass Spectrom. 2016;2:1–10.

    Article  PubMed  Google Scholar 

  12. Dodds JN, Baker ES. Ion mobility spectrometry: fundamental concepts, instrumentation, applications, and the road ahead. J Am Soc Mass Spectrom. 2019;30(11):2185–95.

    Article  PubMed  PubMed Central  CAS  Google Scholar 

  13. Kanu AB, Dwivedi P, Tam M, Matz L, Hill HH. Ion mobility-mass spectrometry. J Mass Spectrom. 2008;43(1):1–22.

    Article  PubMed  CAS  Google Scholar 

  14. Hoaglund CS, Valentine SJ, Sporleder CR, Reilly JP, Clemmer DE. Three-dimensional ion mobility/TOFMS analysis of electrosprayed biomolecules. Anal Chem. 1998;70(11):2236–42.

    Article  PubMed  CAS  Google Scholar 

  15. Wang X, Yu N, Yang J, Jin L, Guo H, Shi W, et al. Suspect and non-target screening of pesticides and pharmaceuticals transformation products in wastewater using QTOF-MS. Environ Int. 2020;137:105599.

    Article  PubMed  CAS  Google Scholar 

  16. Grimm FA, Klaren WD, Li X, Lehmler HJ, Karmakar M, Robertson LW, et al. Cardiovascular effects of polychlorinated biphenyls and their major metabolites. Environ Health Perspect. 2020;128(7):77008.

    Article  PubMed  CAS  Google Scholar 

  17. Dodds JN, Hopkins ZR, Knappe DRU, Baker ES. Rapid characterization of per- and polyfluoroalkyl substances (PFAS) by ion mobility spectrometry-mass spectrometry (IMS-MS). Anal Chem. 2020;92(6):4427–35.

    Article  PubMed  PubMed Central  CAS  Google Scholar 

  18. Baker ES, Clowers BH, Li F, Tang K, Tolmachev AV, Prior DC, et al. Ion mobility spectrometry-mass spectrometry performance using electrodynamic ion funnels and elevated drift gas pressures. J Am Soc Mass Spectrom. 2007;18(7):1176–87.

    Article  PubMed  PubMed Central  CAS  Google Scholar 

  19. Stow SM, Causon TJ, Zheng X, Kurulugama RT, Mairinger T, May JC, et al. An interlaboratory evaluation of drift tube ion mobility-mass spectrometry collision cross section measurements. Anal Chem. 2017;89(17):9048–55.

    Article  PubMed  PubMed Central  CAS  Google Scholar 

  20. Luo YS, Aly NA, McCord J, Strynar MJ, Chiu WA, Dodds JN, et al. Rapid characterization of emerging per- and polyfluoroalkyl substances in aqueous film-forming foams using ion mobility spectrometry-mass spectrometry. Environ Sci Technol. 2020;54(23):15024–34.

    Article  PubMed  PubMed Central  CAS  Google Scholar 

  21. Convention S. All POPs listed in the Stockholm Convention Châtelaine, Switzerland: Stockholm Convention; 2019 [Available from: http://www.pops.int/TheConvention/ThePOPs/AllPOPs/tabid/2509/Default.aspx.

  22. Xiao F. Emerging poly- and perfluoroalkyl substances in the aquatic environment: a review of current literature. Water Res. 2017;124:482–95.

    Article  PubMed  CAS  Google Scholar 

  23. Gluge J, Scheringer M, Cousins IT, DeWitt JC, Goldenman G, Herzke D, et al. An overview of the uses of per- and polyfluoroalkyl substances (PFAS). Environ Sci-Proc Imp. 2020;22(12):2345–73.

    CAS  Google Scholar 

  24. OECD. Synthesis paper on per- and polyfluorinated chemicals (PFCs), environment, health and safety. Environment, Health and Safety Division of the Environment Directorate, OECD: Paris, France; 2013.

    Google Scholar 

  25. Buck RC, Franklin J, Berger U, Conder JM, Cousins IT, de Voogt P, et al. Perfluoroalkyl and polyfluoroalkyl substances in the environment: terminology, classification, and origins. Integr Environ Assess Manag. 2011;7(4):513–41.

    Article  PubMed  PubMed Central  CAS  Google Scholar 

  26. Sunderland EM, Hu XC, Dassuncao C, Tokranov AK, Wagner CC, Allen JG. A review of the pathways of human exposure to poly- and perfluoroalkyl substances (PFASs) and present understanding of health effects. J Expo Sci Environ Epidemiol. 2019;29(2):131–47.

    Article  PubMed  CAS  Google Scholar 

  27. Kosyakov DS, Ul'yanovskii NV, Anikeenko EA, Gorbova NS. Negative ion mode atmospheric pressure ionization methods in lignin mass spectrometry: a comparative study. Rapid Commun Mass Spectrom. 2016;30(19):2099–108.

    Article  PubMed  CAS  Google Scholar 

  28. Zheng X, Dupuis KT, Aly NA, Zhou Y, Smith FB, Tang K, et al. Utilizing ion mobility spectrometry and mass spectrometry for the analysis of polycyclic aromatic hydrocarbons, polychlorinated biphenyls, polybrominated diphenyl ethers and their metabolites. Anal Chim Acta. 2018;1037:265–73.

    Article  PubMed  PubMed Central  CAS  Google Scholar 

  29. US EPA. Learn about polychlorinated biphenyls (PCBs). Washington, D.C.: United States Environmental Protection Agency; 2020 [Available from: https://www.epa.gov/pcbs/learn-about-polychlorinated-biphenyls-pcbs#commercial.

  30. Aslam SN, Huber C, Asimakopoulos AG, Steinnes E, Mikkelsen O. Trace elements and polychlorinated biphenyls (PCBs) in terrestrial compartments of Svalbard. Norwegian Arctic Sci Total Environ. 2019;685:1127–38.

    Article  PubMed  CAS  Google Scholar 

  31. Grimm FA, Hu D, Kania-Korwel I, Lehmler HJ, Ludewig G, Hornbuckle KC, et al. Metabolism and metabolites of polychlorinated biphenyls. Crit Rev Toxicol. 2015;45(3):245–72.

    Article  PubMed  PubMed Central  CAS  Google Scholar 

  32. Guvenius DM, Aronsson A, Ekman-Ordeberg G, Bergman A, Noren K. Human prenatal and postnatal exposure to polybrominated diphenyl ethers, polychlorinated biphenyls, polychlorobiphenylols, and pentachlorophenol. Environ Health Perspect. 2003;111(9):1235–41.

    Article  PubMed  PubMed Central  CAS  Google Scholar 

  33. Herrick RF, Meeker JD, Altshul L. Environmental health indoor exposures, assessments and interventions. Myatt TA, Allen JG, editors. Oakville, ON, CA: Apple Academic Press; 2016.

  34. Espandiari P, Glauert HP, Lehmler HJ, Lee EY, Srinivasan C, Robertson LW. Initiating activity of 4-chlorobiphenyl metabolites in the resistant hepatocyte model. Toxicol Sci. 2004;79(1):41–6.

    Article  PubMed  CAS  Google Scholar 

  35. Grimm FA, Lehmler HJ, He X, Robertson LW, Duffel MW. Sulfated metabolites of polychlorinated biphenyls are high-affinity ligands for the thyroid hormone transport protein transthyretin. Environ Health Perspect. 2013;121(6):657–62.

    Article  PubMed  PubMed Central  Google Scholar 

  36. X.H. Lin JCX, A.A. Keller, L. He, Y.H. Gu, W.W. Zheng, D.Y. Sun, Z.B. Lu, J.W. Huang, X.F. Huang, G.M. Li. Occurrence and risk assessment of emerging contaminants in a water reclamation and ecological reuse project. Sci Total Environ 2020;744.

  37. Hube S, Wu B. Mitigation of emerging pollutants and pathogens in decentralized wastewater treatment processes: a review. Sci Total Environ. 2021;779:146545.

    Article  PubMed  CAS  Google Scholar 

  38. Vajda AM, Barber LB, Gray JL, Lopez EM, Bolden AM, Schoenfuss HL, et al. Demasculinization of male fish by wastewater treatment plant effluent. Aquat Toxicol. 2011;103(3–4):213–21.

    Article  PubMed  CAS  Google Scholar 

  39. Guiloski IC, Ribas JLC, Piancini LDS, Dagostim AC, Cirio SM, Favaro LF, et al. Paracetamol causes endocrine disruption and hepatotoxicity in male fish Rhamdia quelen after subchronic exposure. Environ Toxicol Pharmacol. 2017;53:111–20.

    Article  PubMed  CAS  Google Scholar 

  40. Lv YZ, Yao L, Wang L, Liu WR, Zhao JL, He LY, et al. Bioaccumulation, metabolism, and risk assessment of phenolic endocrine disrupting chemicals in specific tissues of wild fish. Chemosphere. 2019;226:607–15.

    Article  PubMed  CAS  Google Scholar 

  41. Plasencia MD, Isailovic D, Merenbloom SI, Mechref Y, Novotny MV, Clemmer DE. Resolving and assigning N-linked glycan structural isomers from ovalbumin by IMS-MS. J Am Soc Mass Spectrom. 2008;19(11):1706–15.

    Article  PubMed  PubMed Central  CAS  Google Scholar 

  42. Isailovic D, Kurulugama RT, Plasencia MD, Stokes ST, Kyselova Z, Goldman R, et al. Profiling of human serum glycans associated with liver cancer and cirrhosis by IMS-MS. J Proteome Res. 2008;7(3):1109–17.

    Article  PubMed  PubMed Central  CAS  Google Scholar 

  43. Sim WJ, Lee JW, Lee ES, Shin SK, Hwang SR, Oh JE. Occurrence and distribution of pharmaceuticals in wastewater from households, livestock farms, hospitals and pharmaceutical manufactures. Chemosphere. 2011;82(2):179–86.

    Article  PubMed  CAS  Google Scholar 

  44. Zhang W, Pang S, Lin Z, Mishra S, Bhatt P, Chen S. Biotransformation of perfluoroalkyl acid precursors from various environmental systems: advances and perspectives. Environ Pollut. 2021;272:115908.

    Article  PubMed  CAS  Google Scholar 

  45. Schaefer CE, Choyke S, Ferguson PL, Andaya C, Burant A, Maizel A, et al. Electrochemical transformations of perfluoroalkyl acid (PFAA) precursors and PFAAs in groundwater impacted with aqueous film forming foams. Environ Sci Technol. 2018;52(18):10689–97.

    Article  PubMed  CAS  Google Scholar 

  46. Liu JX, Avendano SM. Microbial degradation of polyfluoroalkyl chemicals in the environment: a review. Environ Int. 2013;61:98–114.

    Article  PubMed  CAS  Google Scholar 

  47. Shaw DMJ, Munoz G, Bottos EM, Duy SV, Sauve S, Liu J, et al. Degradation and defluorination of 6:2 fluorotelomer sulfonamidoalkyl betaine and 6:2 fluorotelomer sulfonate by Gordonia sp. strain NB4-1Y under sulfur-limiting conditions. Sci Total Environ. 2019;647:690–8.

    Article  PubMed  CAS  Google Scholar 

  48. Singh RK, Fernando S, Baygi SF, Multari N, Thagard SM, Holsen TM. Breakdown products from perfluorinated alkyl substances (PFAS) degradation in a plasma-based water treatment process. Environ Sci Technol. 2019;53(5):2731–8.

    Article  PubMed  CAS  Google Scholar 

  49. Aly NA, Luo YS, Liu Y, Casillas G, McDonald TJ, Kaihatu JM, et al. Temporal and spatial analysis of per and polyfluoroalkyl substances in surface waters of Houston ship channel following a large-scale industrial fire incident. Environ Pollut. 2020;265(Pt B):115009.

    Article  PubMed  PubMed Central  CAS  Google Scholar 

Download references

Acknowledgements

This work was funded, in part, by grants from the National Institutes of Health (P30 ES025128, P42 ES027704, and P42 ES031009) and a cooperative agreement with the United States Environmental Protection Agency (STAR RD 84003201). The views expressed in this manuscript do not reflect those of the funding agencies. The use of specific commercial products in this work does not constitute endorsement by the authors or the funding agencies.

Author information

Author notes

  1. Yu-Syuan Luo

    Present address: Institute of Food Safety and Health, College of Public Health, National Taiwan University, Taipei, Taiwan

Authors and Affiliations

  1. Interdisciplinary Faculty of Toxicology, Texas A&M University, College Station, TX, USA

    Noor A. Aly, Yu-Syuan Luo, Fabian A. Grimm & Ivan Rusyn

  2. Department of Veterinary Integrative Biosciences, Texas A&M University, College Station, TX, USA

    Noor A. Aly, Yu-Syuan Luo, Fabian A. Grimm & Ivan Rusyn

  3. Department of Chemistry, North Carolina State University, Raleigh, NC, USA

    James N. Dodds, MaKayla Foster & Erin S. Baker

Authors
  1. Noor A. Aly
    View author publications

    You can also search for this author in PubMed Google Scholar

  2. James N. Dodds
    View author publications

    You can also search for this author in PubMed Google Scholar

  3. Yu-Syuan Luo
    View author publications

    You can also search for this author in PubMed Google Scholar

  4. Fabian A. Grimm
    View author publications

    You can also search for this author in PubMed Google Scholar

  5. MaKayla Foster
    View author publications

    You can also search for this author in PubMed Google Scholar

  6. Ivan Rusyn
    View author publications

    You can also search for this author in PubMed Google Scholar

  7. Erin S. Baker
    View author publications

    You can also search for this author in PubMed Google Scholar

Corresponding author

Correspondence to Erin S. Baker.

Ethics declarations

Competing interests

The authors declare no competing interests.

Additional information

Published in the topical collection Per- and Polyfluoroalkyl Substances (PFAS)– Contaminants of Emerging Concern with guest editors Erin Baker and Detlef Knappe.

Publisher’s note

Springer Nature remains neutral with regard to jurisdictional claims in published maps and institutional affiliations.

Supplementary information

ESM 1

(DOCX 12 kb)

ESM 2

(XLSX 32 kb)

Rights and permissions

Reprints and permissions

About this article

Check for updates. Verify currency and authenticity via CrossMark

Cite this article

Aly, N.A., Dodds, J.N., Luo, YS. et al. Utilizing ion mobility spectrometry-mass spectrometry for the characterization and detection of persistent organic pollutants and their metabolites. Anal Bioanal Chem 414, 1245–1258 (2022). https://doi.org/10.1007/s00216-021-03686-w

Download citation

  • Received:

  • Revised:

  • Accepted:

  • Published:

  • Issue Date:

  • DOI: https://doi.org/10.1007/s00216-021-03686-w

Keywords

Search

Navigation