Detection of N-nitrosodimethylamine (NDMA) and its formation potential in hospital wastewater

Abstract

Hospital wastewaters contain high concentrations of pharmaceutical residues and other chemicals, and may present an important source for NDMA (N-nitrosodimethylamine) and its precursors in the aquatic environment. The present study evaluates the contribution of hospital wastewater to NDMA environmental load and identifies important sources within the hospital itself. For this purpose, wastewaters from five large hospitals in Israel were analyzed, and concentrations of NDMA were found in the range of 20.7–56.7 ng/L, which are similar to NDMA concentrations typically detected in domestic wastewater. The relative contribution of day surgery, oncology, laboratories, and central kitchen (in Sheba hospital) to the daily load of NDMA was calculated as 20.2%, 8.2%, 10%, and 43.2%, respectively. In addition, NDMA concentration in Sheba’s mixed wastewater stream, measured throughout a complete working day, was highest at 14:00. This suggests the possible impact of lunchtime on NDMA concentration, and emphasizes the dominant contribution of central kitchen waste. Finally, formation potential of NDMA in the mixed stream was 7300 ng/L, in the upper range of domestic wastewater, but could be decreased by 70% during subsequent aerobic biological wastewater treatment.

This is a preview of subscription content, access via your institution.

Fig. 1
Fig. 2
Fig. 3

References

  1. APHA (2005) Standard Methods for the Examination of Water & Wastewater, 21st ed. American Public Health Association (APHA)/American Water Works Association/Water Environment Federation, Washington, DC, USA

  2. Bian Y, Wang C, Zhu G, Ren B, Zhang P, Hursthouse AS (2019) Occurrence and control of N-nitrosodimethylamine in water engineering systems. Environ Eng Res 24:1–16. https://doi.org/10.4491/eer.2018.021

    Article  Google Scholar 

  3. Duong HA, Pham NH, Nguyen HT, Hoang TT, Pham HV, Pham VC, Berg M, Giger W, Alder AC (2008) Occurrence, fate and antibiotic resistance of fluoroquinolone antibacterials in hospital wastewaters in Hanoi, Vietnam. Chemosphere 72:968–973. https://doi.org/10.1016/j.chemosphere.2008.03.009

    CAS  Article  Google Scholar 

  4. Garland WA, Kuenzig W, Rubio F, Kornychuk H, Conney AH (1986) Urinary excretion of nitrosodimethylamine and nitrosoproline in humans: interindividual and intraindividual differences and the effect of administered ascorbic acid and α-tocopherol. Cancer Res 46:5392–5400

    CAS  Google Scholar 

  5. Gómez MJ, Petrović M, Fernández-Alba AR, Barceló D (2006) Determination of pharmaceuticals of various therapeutic classes by solid-phase extraction and liquid chromatography-tandem mass spectrometry analysis in hospital effluent wastewaters. J Chromatogr A 1114:224–233. https://doi.org/10.1016/j.chroma.2006.02.038

    CAS  Article  Google Scholar 

  6. Guyer JP (2010) Introduction to hydraulic design of sewers

  7. Heberer T, Feldmann D (2005) Contribution of effluents from hospitals and private households to the total loads of diclofenac and carbamazepine in municipal sewage effluents - modeling versus measurements. J Hazard Mater 122:211–218. https://doi.org/10.1016/j.jhazmat.2005.03.007

    CAS  Article  Google Scholar 

  8. Helwig K, Hunter C, Mcnaughtan M, Roberts J, Pahl O (2016) Ranking prescribed pharmaceuticals in terms of environmental risk: inclusion of hospital data and the importance of regular review. Environ Toxicol Chem 35:1043–1050. https://doi.org/10.1002/etc.3302

    CAS  Article  Google Scholar 

  9. Kosaka K, Asami M, Ohkubo K, Iwamoto T, Tanaka Y, Koshino H, Echigo S, Akiba M (2014) Identification of a New N-nitrosodimethylamine precursor in sewage containing industrial effluents. Environ Sci Technol 48:11243–11250. https://doi.org/10.1021/es502284t

    CAS  Article  Google Scholar 

  10. Krasner SW, Mitch WA, McCurry DL, Hanigan D, Westerhoff P (2013) Formation, precursors, control, and occurrence of nitrosamines in drinking water: A review. Water Res 47:4433–4450. https://doi.org/10.1016/j.watres.2013.04.050

    CAS  Article  Google Scholar 

  11. Kümmerer K (2001) Drugs in the environment: emission of drugs, diagnostic aids and disinfectants into wastewater by hospitals in relation to other sources - A review. Chemosphere 45:957–969. https://doi.org/10.1016/S0045-6535(01)00144-8

    Article  Google Scholar 

  12. Le Roux J, Gallard H, Croué JP (2011) Chloramination of nitrogenous contaminants (pharmaceuticals and pesticides): NDMA and halogenated DBPs formation. Water Res 45:3164–3174. https://doi.org/10.1016/j.watres.2011.03.035

    CAS  Article  Google Scholar 

  13. Le Roux J, Gallard H, Croué JP (2012) Formation of NDMA and halogenated DBPs by chloramination of tertiary amines: The influence of bromide ion. Environ Sci Technol 46:1581–1589. https://doi.org/10.1021/es203785s

    CAS  Article  Google Scholar 

  14. Lindberg R, Jarnheimer PÅ, Olsen B, Johansson M, Tysklind M (2004) Determination of antibiotic substances in hospital sewage water using solid phase extraction and liquid chromatography/mass spectrometry and group analogue internal standards. Chemosphere 57:1479–1488. https://doi.org/10.1016/j.chemosphere.2004.09.015

    CAS  Article  Google Scholar 

  15. Ma F, Wan Y, Yuan G, Meng L, Dong Z, Hu J (2012) Occurrence and source of nitrosamines and secondary amines in groundwater and its adjacent Jialu River Basin, China. Environ Sci Technol 46:3236–3243. https://doi.org/10.1021/es204520b

    CAS  Article  Google Scholar 

  16. Mamo J, Insa S, Monclús H, Rodríguez-Roda I, Comas J, Barceló D, Farré MJ (2016) Fate of NDMA precursors through an MBR-NF pilot plant for urban wastewater reclamation and the effect of changing aeration conditions. Water Res 102:383–393. https://doi.org/10.1016/j.watres.2016.06.057

    CAS  Article  Google Scholar 

  17. Mayoudom EVT, Nguidjoe E, Mballa RN, Tankoua OF, Fokunang C, Anyakora C, Blackett KN (2018) Identification and quantification of 19 pharmaceutical active compounds and metabolites in hospital wastewater in Cameroon using LC/QQQ and LC/Q-TOF. Environ Monit Assess 190:1–10. https://doi.org/10.1007/s10661-018-7097-1

    CAS  Article  Google Scholar 

  18. Mitch WA, Sedlak DL (2002) Formation of N-nitrosodimethylamine (NDMA) from dimethylamine during chlorination. Environ Sci Technol 36:588–595. https://doi.org/10.1021/es010684q

    CAS  Article  Google Scholar 

  19. Mitch WA, Sedlak DL (2004) Characterization and fate of N-nitrosodimethylamine precursors in municipal wastewater treatment plants. Environ Sci Technol 38:1445–1454. https://doi.org/10.1021/es035025n

    CAS  Article  Google Scholar 

  20. Mitch WA, Sharp JO, Trussell RR, Valentine RL, Alvarez-Cohen L, Sedlak DL (2003) N-Nitrosodimethylamine (NDMA) as a drinking water contaminant: a review. Environ Eng Sci 20:389–404. https://doi.org/10.1089/109287503768335896

    CAS  Article  Google Scholar 

  21. Ohlsen K, Ternes T, Werner G, Wallner U, Löffler D, Ziebuhr W, Witte W, Hacker J (2003) Impact of antibiotics on conjugational resistance gene transfer in Staphylococcus aureus in sewage. Environ Microbiol 5:711–716. https://doi.org/10.1046/j.1462-2920.2003.00459.x

    CAS  Article  Google Scholar 

  22. Poustie A (2018) Quantification of trace anthropogenic compounds in reclaimed wastewater, M.sc. thesis, University of Nevada, Reno

  23. Richardson SD, Ternes TA (2018) Water analysis: emerging contaminants and current issues. Anal Chem 90:398–428. https://doi.org/10.1021/acs.analchem.7b04577

    CAS  Article  Google Scholar 

  24. Schmidt CK, Brauch HJ (2008) N,N-dimethylsulfamide as precursor for N-nitrosodimethylamine (NDMA) formation upon ozonation and its fate during drinking water treatment. Environ Sci Technol 42:6340–6346. https://doi.org/10.1021/es7030467

    CAS  Article  Google Scholar 

  25. Schreiber IM, Mitch WA (2006) Nitrosamine formation pathway revisited: the importance of chloramine speciation and dissolved oxygen. Environ Sci Technol 40:6007–6014. https://doi.org/10.1021/es060978h

    CAS  Article  Google Scholar 

  26. Schreiber IM, Mitch WA (2008) Degradation of tertiary alkylamines during chlorination/chloramination : implications for formation of. Environ Sci Technol 42:4811–4817

    Article  Google Scholar 

  27. Sedlak DL, Deeb RA, Hawley EL, Mitch WA, Durbin TD, Mowbray S, Carr S (2005) Sources and fate of nitrosodimethylamine and its precursors in municipal wastewater treatment plants. Water Environ Res 77:32–39. https://doi.org/10.2175/106143005x41591

    CAS  Article  Google Scholar 

  28. Selbes M, Kim D, Ates N, Karanfil T (2013) The roles of tertiary amine structure, background organic matter and chloramine species on NDMA formation. Water Res 47:945–953. https://doi.org/10.1016/j.watres.2012.11.014

    CAS  Article  Google Scholar 

  29. Serna-Galvis EA, Silva-Agredo J, Botero-Coy AM, Moncayo-Lasso A, Hernández F, Torres-Palma RA (2019) Effective elimination of fifteen relevant pharmaceuticals in hospital wastewater from Colombia by combination of a biological system with a sonochemical process. Sci Total Environ 670:623–632. https://doi.org/10.1016/j.scitotenv.2019.03.153

    CAS  Article  Google Scholar 

  30. Sgroi M, Vagliasindi FGA, Snyder SA, Roccaro P (2018) N-Nitrosodimethylamine (NDMA) and its precursors in water and wastewater: a review on formation and removal. Chemosphere 191:685–703. https://doi.org/10.1016/j.chemosphere.2017.10.089

    CAS  Article  Google Scholar 

  31. Shen R, Andrews SA (2011a) NDMA formation kinetics from three pharmaceuticals in four water matrices. Water Res 45:5687–5694. https://doi.org/10.1016/j.watres.2011.08.034

    CAS  Article  Google Scholar 

  32. Shen R, Andrews SA (2011b) Demonstration of 20 pharmaceuticals and personal care products (PPCPs) as nitrosamine precursors during chloramine disinfection. Water Res 45:944–952. https://doi.org/10.1016/j.watres.2010.09.036

    CAS  Article  Google Scholar 

  33. Souza FS, Féris LA (2016) Hospital and municipal wastewater: identification of relevant pharmaceutical compounds. Water Environ Res 88:871–877. https://doi.org/10.2175/106143016x14609975747603

    CAS  Article  Google Scholar 

  34. USEPA (2004) Method 521: Determination of nitrosamines in drinking water by solid phase extraction and capillary column gas chromatography with large volume injection and chemical ionization tandem mass spectrometry (MS/MS). Epa/600/R-05/054; 2004 I:1–47

  35. Verlicchi P, Galletti A, Petrovic M, BarcelÓ D (2010) Hospital effluents as a source of emerging pollutants: an overview of micropollutants and sustainable treatment options. J Hydrol 389:416–428. https://doi.org/10.1016/j.jhydrol.2010.06.005

    CAS  Article  Google Scholar 

  36. Wang L, Li Y, He G (2014a) Degradation of typical N-nitrosodimethylamine (NDMA) precursors and its formation potential in anoxic-aerobic (AO) activated sludge system. J Environ Sci Heal - Part A Toxic/Hazardous Subst Environ Eng 49:1727–1739. https://doi.org/10.1080/10934529.2014.951263

    CAS  Article  Google Scholar 

  37. Wang L, Li Y, Shang X, Shen J (2014b) Occurrence and removal of N-nitrosodimethylamine and its precursors in wastewater treatment plants in and around Shanghai. Front Environ Sci Eng 8:519–530. https://doi.org/10.1007/s11783-013-0610-4

    CAS  Article  Google Scholar 

  38. Woods GC, Dickenson ERV (2015) Evaluation of the final UCMR2 database: nationwide trends in NDMA. J Am Water Works Assoc 107:E58–E68. https://doi.org/10.5942/jawwa.2015.107.0009

    Article  Google Scholar 

  39. Woods-Chabane GC, Glover CM, Marti EJ, Dickenson ERV (2017) A novel assay to measure tertiary and quaternary amines in wastewater: an indicator for NDMA wastewater precursors. Chemosphere 179:298–305. https://doi.org/10.1016/j.chemosphere.2017.03.045

    CAS  Article  Google Scholar 

  40. Yang L, Chen Z, Shen J, Xu Z, Liang H, Tian J, Ben Y, Zhai X, Shi W, Li G (2009) Reinvestigation of the nitrosamine-formation mechanism during ozonation. Environ Sci Technol 43:5481–5487. https://doi.org/10.1021/es900319f

    CAS  Article  Google Scholar 

  41. Zeng T, Mitch WA (2015) Contribution of N-nitrosamines and their precursors to domestic sewage by greywaters and blackwaters. Environ Sci Technol 49:13158–13167. https://doi.org/10.1021/acs.est.5b04254

    CAS  Article  Google Scholar 

  42. Zeng T, Glover CM, Marti EJ, Woods-Chabane GC, Karanfil T, Mitch WA, Dickenson ERV (2016) Relative importance of different water categories as sources of N-nitrosamine precursors. Environ Sci Technol 50:13239–13248. https://doi.org/10.1021/acs.est.6b04650

    CAS  Article  Google Scholar 

Download references

Acknowledgements

We would like to thank Adi Zilberman for her work in the biological wastewater treatment system and to Dr. Igal Gozlan for his guide on the GCMS method adjustment.

Availability of data and materials

All data generated or analyzed during this study are included in this published article.

Funding

The study was partially funded by the Azrieli College research fund.

Author information

Affiliations

Authors

Contributions

SS carried out all the fieldwork, including sampling wastewaters from the different hospitals, and was a major contributor in writing the manuscript. DA assisted with the analytical methods. AK operated the GC-MS. YL designed and managed the entire study. All authors read and approved the final manuscript.

Corresponding author

Correspondence to Yaal Lester.

Ethics declarations

Ethics approval and consent to participate

Not applicable.

Consent for publication

Not applicable.

Competing interests

The authors declare that they have no competing interests.

Additional information

Publisher’s note

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

Responsible Editor: Ester Heath

Supplementary information

ESM 1

(DOC 35 kb)

Rights and permissions

Reprints and Permissions

About this article

Verify currency and authenticity via CrossMark

Cite this article

Sack, S., Avisar, D., Kaplan, A. et al. Detection of N-nitrosodimethylamine (NDMA) and its formation potential in hospital wastewater. Environ Sci Pollut Res (2021). https://doi.org/10.1007/s11356-021-12785-1

Download citation

Keywords

  • Hospital wastewaters
  • NDMA
  • Formation potential
  • Biological treatment