Influence of Metal Speciation in Wastewater Sludge on Antibiotic Distribution
Publication: Journal of Hazardous, Toxic, and Radioactive Waste
Volume 25, Issue 2
Abstract
The analytical study was conducted to evaluate the concentration of ciprofloxacin (CIP), chlortetracycline (CTC), and chosen metals in a wastewater treatment plant. The concentration of CIP was slightly higher in the effluent (0.703 ± 0.045 µg/L) than the influent (0.467 ± 0.049 µg/L) in wastewater samples. More than 70% of CTC was recovered during wastewater treatment; its concentration in wastewater effluent was at 6.13 ± 0.863 µg/L. High concentration of CIP and CTC, 3.9 and 11 mg/kg, respectively, were detected in the solid fractions of sludge. This elevated concentration might have been due to interactions with metals in sludge (i.e., 64–89 g/kg of Ca, 52–109 g/kg of Fe) as both antibiotics have the capacity to form complexes with them. The chemical speciation of all sludge types was carried out to further investigate the distribution of targeted metals and antibiotics and to establish if there is any interdependence. The positive correlation between CTC/CIP concentration and Mg, Ca, and As concentration in primary sludge was observed. This suggests that metal-antibiotic interaction may contribute to primary wastewater treatment.
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Acknowledgments
The authors are sincerely thankful to the Natural Sciences and Engineering Research Council of Canada (Discovery Grant 355254 and NSERC Strategic Grant). We would like to also thank Mr. Stephane Moise for his technical support with Liquid Chromatography analysis. We would like to thank Dr. Manjit Singh Rana for his critical readings and comments.
References
Álvarez, E. A., M. C. Mochón, J. C. J. Sánchez, and M. T. Rodrìguez. 2002. “Heavy metal extractable forms in sludge from wastewater treatment plants.” Chemosphere 47 (7): 765–775. https://doi.org/10.1016/S0045-6535(02)00021-8.
Amarakoon, I. D., F. Zvomuya, A. J. Cessna, D. Degenhardt, F. J. Larney, and T. A. McAllister. 2014. “Runoff losses of excreted chlortetracycline, sulfamethazine, and tylosin from surface-applied and soil-incorporated beef cattle feedlot manure.” J. Environ. Qual. 43 (2): 549–557. https://doi.org/10.2134/jeq2013.02.0039.
APHA, AWWA, WEF (American Public Health Association, American Water Works Association, Water Environment Federation). 2005. Vol. 21 of Standard methods for the examination of water and wastewater, 258–259. Washington, DC: APHA, AWWA, WEF.
Archana, G., R. Dhodapkar, and A. Kumar. 2016. “Offline solid-phase extraction for preconcentration of pharmaceuticals and personal care products in environmental water and their simultaneous determination using the reversed phase high-performance liquid chromatography method.” Environ. Monit. Assess. 188 (9): 512. https://doi.org/10.1007/s10661-016-5510-1.
Aristilde, L., and G. Sposito. 2010. “Binding of ciprofloxacin by humic substances: A molecular dynamics study.” Environ. Toxicol. Chem. 29 (1): 90–98. https://doi.org/10.1002/etc.19.
Ashraf, M., M. Maah, and I. Yusoff. 2012. “Chemical speciation and potential mobility of heavy metals in the soil of former tin mining catchment.” Sci. World J. 2012: 125608. https://doi.org/10.1100/2012/125608.
Cheng, M., L. Wu, Y. Huang, Y. Luo, and P. Christie. 2014. “Total concentrations of heavy metals and occurrence of antibiotics in sewage sludges from cities throughout China.” J. Soils Sediments 14 (6): 1123–1135. https://doi.org/10.1007/s11368-014-0850-3.
Cuprys, A., R. Pulicharla, S. K. Brar, P. Drogui, M. Verma, and R. Y. Surampalli. 2018a. “Fluoroquinolones metal complexation and its environmental impacts.” Coord. Chem. Rev. 376: 46–61. https://doi.org/10.1016/j.ccr.2018.05.019.
Cuprys, A., R. Pulicharla, J. Lecka, S. K. Brar, P. Drogui, and R. Y. Surampalli. 2018b. “Ciprofloxacin-metal complexes -stability and toxicity tests in the presence of humic substances.” Chemosphere 202: 549–559. https://doi.org/10.1016/j.chemosphere.2018.03.117.
Dong, B., X. Liu, L. Dai, and X. Dai. 2013. “Changes of heavy metal speciation during high-solid anaerobic digestion of sewage sludge.” Bioresour. Technol. 131: 152–158. https://doi.org/10.1016/j.biortech.2012.12.112.
Fuentes, A., M. Lloréns, J. Sáez, M. I. Aguilar, J. F. Ortuño, and V. F. Meseguer. 2004. “Phytotoxicity and heavy metals speciation of stabilised sewage sludges.” J. Hazard. Mater. 108 (3): 161–169. https://doi.org/10.1016/j.jhazmat.2004.02.014.
Gaugain, M., S. Gautier, S. Bourcier, A.-M. Jacques, M. Laurentie, J.-P. Abjean, D. Hurtaud-Pessel, and E. Verdon. 2015. “6-Iso-chlortetracycline or keto form of chlortetracycline? Need for clarification for relevant monitoring of chlortetracycline residues in food.” Food Addit. Contam., Part A 32 (7): 1105–1115. https://doi.org/10.1080/19440049.2015.1036381.
Gu, C., and K. G. Karthikeyan. 2005. “Sorption of the antimicrobial ciprofloxacin to aluminum and iron hydrous oxides.” Environ. Sci. Technol. 39 (23): 9166–9173. https://doi.org/10.1021/es051109f.
Jia, A., Y. Wan, Y. Xiao, and J. Hu. 2012. “Occurrence and fate of quinolone and fluoroquinolone antibiotics in a municipal sewage treatment plant.” Water Res. 46 (2): 387–394. https://doi.org/10.1016/j.watres.2011.10.055.
Larsson, D. J. 2014. “Antibiotics in the environment.” Upsala J. Med. Sci. 119 (2): 108–112. https://doi.org/10.3109/03009734.2014.896438.
Lee, H. B., T. E. Peart, and M. L. Svoboda. 2007. “Determination of ofloxacin, norfloxacin, and ciprofloxacin in sewage by selective solid-phase extraction, liquid chromatography with fluorescence detection, and liquid chromatography–tandem mass spectrometry.” J. Chromatogr. A 1139 (1): 45–52. https://doi.org/10.1016/j.chroma.2006.11.068.
Li, B., and T. Zhang. 2010. “Biodegradation and adsorption of antibiotics in the activated sludge process.” Environ. Sci. Technol. 44 (9): 3468–3473. https://doi.org/10.1021/es903490h.
Li, N., X. Zhang, W. Wu, and X. Zhao. 2014. “Occurrence, seasonal variation and risk assessment of antibiotics in the reservoirs in North China.” Chemosphere 111: 327–335. https://doi.org/10.1016/j.chemosphere.2014.03.129.
Liang, X., X.-a. Ning, G. Chen, M. Lin, J. Liu, and Y. Wang. 2013. “Concentrations and speciation of heavy metals in sludge from nine textile dyeing plants.” Ecotoxicol. Environ. Saf. 98: 128–134. https://doi.org/10.1016/j.ecoenv.2013.09.012.
Miao, X. S., F. Bishay, M. Chen, and C. D. Metcalfe. 2004. “Occurrence of antimicrobials in the final effluents of wastewater treatment plants in Canada.” Environ. Sci. Technol. 38 (13): 3533–3541. https://doi.org/10.1021/es030653q.
Nilsen, E., K. L. Smalling, L. Ahrens, M. Gros, K. S. B. Miglioranza, Y. Picó, and H. L. Schoenfuss. 2019. “Critical review: Grand challenges in assessing the adverse effects of contaminants of emerging concern on aquatic food webs.” Environ. Toxicol. Chem. 38 (1): 46–60. https://doi.org/10.1002/etc.4290.
Noguera-Oviedo, K., and D. S. Aga. 2016. “Lessons learned from more than two decades of research on emerging contaminants in the environment.” J. Hazard. Mater. 316: 242–251. https://doi.org/10.1016/j.jhazmat.2016.04.058.
Östman, M., R. H. Lindberg, J. Fick, E. Björn, and M. Tysklind. 2017. “Screening of biocides, metals and antibiotics in Swedish sewage sludge and wastewater.” Water Res. 115: 318–328. https://doi.org/10.1016/j.watres.2017.03.011.
PHAC (Public Health Agency of Canada). 2018. Canadian antimicrobial resistance surveillance system update 2018. Ottawa: PHAC.
Pulicharla, R., R. K. Das, S. K. Brar, P. Drogui, S. J. Sarma, M. Verma, R. Y. Surampalli, and J. R. Valero. 2015. “Toxicity of chlortetracycline and its metal complexes to model microorganisms in wastewater sludge.” Sci. Total Environ. 532: 669–675. https://doi.org/10.1016/j.scitotenv.2015.05.140.
Pulicharla, R., K. Hegde, S. K. Brar, and R. Y. Surampalli. 2017. “Tetracyclines metal complexation: Significance and fate of mutual existence in the environment.” Environ. Pollut. 221: 1–14. https://doi.org/10.1016/j.envpol.2016.12.017.
Puicharla, R., D. P. Mohapatra, S. K. Brar, P. Drogui, S. Auger, and R. Y. Surampalli. 2014. “A persistent antibiotic partitioning and co-relation with metals in wastewater treatment plant—Chlortetracycline.” J. Environ. Chem. Eng. 2 (3): 1596–1603. https://doi.org/10.1016/j.jece.2014.06.001.
Rajaganapathy, V., F. Xavier, D. Sreekumar, and P. Mandal. 2011. “Heavy metal contamination in soil, water and fodder and their presence in livestock and products : A review.” J. Environ. Sci. Technol. 4 (3): 234–249. https://doi.org/10.3923/jest.2011.234.249.
Sharma, C., N. Rokana, M. Chandra, B. P. Singh, R. D. Gulhane, J. P. S. Gill, P. Ray, A. K. Puniya, and H. Panwar. 2018. “Antimicrobial resistance: Its surveillance, impact, and alternative management strategies in dairy animals.” Front. Vet. Sci. 4: 237. https://doi.org/10.3389/fvets.2017.00237.
Suresh, G., R. K. Das, S. Kaur Brar, T. Rouissi, A. Avalos Ramirez, Y. Chorfi, and S. Godbout. 2018. “Alternatives to antibiotics in poultry feed: Molecular perspectives.” Crit. Rev. Microbiol. 44 (3): 318–335. https://doi.org/10.1080/1040841X.2017.1373062.
Urbaniak, B., and Z. J. Kokot. 2009. “Analysis of the factors that significantly influence the stability of fluoroquinolone-metal complexes.” Anal. Chim. Acta 647 (1): 54–59. https://doi.org/10.1016/j.aca.2009.05.039.
USFDA (U.S. Food and Drug Administration). 2017. 2016 summary report on antimicrobials sold or distributed for use in food-producing animals. Washington, DC: U.S. Food and Drug Administration, Center for veterinary medicine.
Van Doorslaer, X., J. Dewulf, H. Van Langenhove, and K. Demeestere. 2014. “Fluoroquinolone antibiotics: An emerging class of environmental micropollutants.” Sci. Total Environ. 500–501: 250–269. https://doi.org/10.1016/j.scitotenv.2014.08.075.
Wei, B., and L. Yang. 2010. “A review of heavy metal contaminations in urban soils, urban road dusts and agricultural soils from China.” Microchem. J. 94 (2): 99–107. https://doi.org/10.1016/j.microc.2009.09.014.
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Journal of Hazardous, Toxic, and Radioactive Waste
Volume 25 • Issue 2 • April 2021
Copyright
© 2020 American Society of Civil Engineers.
History
Received: Jul 18, 2020
Accepted: Oct 20, 2020
Published online: Dec 9, 2020
Published in print: Apr 1, 2021
Discussion open until: May 9, 2021
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