Abstract
Pharmaceuticals are chemical compounds employed as medicinal drugs. They have severe physic-chemical properties which make them destructive for non-target species. Consequently, their continuous addition in the environment may pose hazardous effects. Among these, diclofenac (DCF), a non-steroidal anti-inflammatory drug (NSAID), is extensively used in Pakistan which may lead to its accumulation in both terrestrial and aquatic environment. Present study aims to assess the presence and concentration of pharmaceutically active drug (DCF) in surface water and wastewater of twin cities of Pakistan (Rawalpindi and Islamabad). For this purpose, a validated high-performance liquid chromatography (HPLC) method was adopted involving solid-phase extraction procedure. Wastewater samples were collected from various sites of Rawalpindi and Islamabad. Results of HPLC analysis revealed that DCF was extant with considerably high concentration, not only in wastewater but also in surface water samples. Concentrations as high as 216 μg L−1 was detected in Rawat industrial area and low as 8 μg L−1 was detected in dairy farm wastewater samples collected from Taramri. However, maximum DCF levels in residential wastewater and hospital wastewater were detected to be 105 μg L−1 and 34 μg L−1, respectively. Moreover, the highest detected level (116 μg L−1) was found in surface water of Sawan River. Further, results of ecological risk assessment revealed its possible toxic effects of DCF on various aquatic organisms.
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Ashfaq, M., Khan, K. N., Rehman, M. S. U., Mustafa, G., Nazar, M. F., Sun, Q., & Yu, C. P. (2017a). Ecological risk assessment of pharmaceuticals in the receiving environment of pharmaceutical wastewater in Pakistan. Ecotoxicology and Environmental Safety, 136, 31–39.
Ashfaq, M., Noor, N., Saif-Ur-Rehman, M., Sun, Q., Mustafa, G., Faizan Nazar, M., & Yu, C. P. (2017b). Determination of commonly used pharmaceuticals in hospital waste of Pakistan and evaluation of their ecological risk assessment. CLEAN–Soil, Air, Water, 45(6), 1500392.
Bouissou-Schurtz, C., Houeto, P., Guerbet, M., Bachelot, M., Casellas, C., Mauclaire, A. C., & Masset, D. (2014). Ecological risk assessment of the presence of pharmaceutical residues in a French national water survey. Regulatory Toxicology and Pharmacology, 69(3), 296–303.
Bound, J. P., & Voulvoulis, N. (2004). Pharmaceuticals in the aquatic environment––a comparison of risk assessment strategies. Chemosphere, 56(11), 1143–1155.
Carmona, E., Andreu, V., & Picó, Y. (2014). Occurrence of acidic pharmaceuticals and personal care products in Turia River Basin: from waste to drinking water. Science of the Total Environment, 484, 53–63.
Ericson, H., Thorsen, G., & Kumblad, L. (2010). Physiological effects of diclofenac, ibuprofen and propranolol on Baltic Sea blue mussels. Aquatic Toxicology., 99, 223–231.
Escher, B. I., Baumgartner, R., Koller, M., Treyer, K., Lienert, J., & McArdell, C. S. (2011). Environmental toxicology and risk assessment of pharmaceuticals from hospital wastewater. Water Research, 45(1), 75–92.
Feito, R., Valcárcel, Y., & Catalá, M. (2012). Biomarker assessment of toxicity with miniaturised bioassay: diclofenac as a case study. Ecotoxicology, 21, 289–296.
Guiloski, I. C., Piancini, L. D. S., Dagostim, A. C., de Morais Calado, S. L., Fávaro, L. F., Boschen, S. L., & de Assis, H. C. S. (2017). Effects of environmentally relevant concentrations of the anti-inflammatory drug diclofenac in freshwater fish Rhamdia quelen. Ecotoxicology and Environmental Safety, 139, 291–300.
Haap, T., Triebskorn, R., & Köhler, H. R. (2008). Acute effects of diclofenac and DMSO to Daphnia magna: immobilisation and hsp70-induction. Chemosphere, 73(3), 353–359.
Han, G. H., Hur, H. G., & Kim, S. D. (2006). Ecotoxicological risk of pharmaceuticals from wastewater treatment plants in Korea: occurrence and toxicity to Daphnia magna. Environmental Toxicology and Chemistry: An International Journal, 25(1), 265–271.
Hernando, M. D., Mezcua, M., Fernández-Alba, A. R., & Barceló, D. (2006). Environmental risk assessment of pharmaceutical residues in wastewater effluents, surface waters and sediments. Talanta, 69(2), 334–342.
Hu, J., Zhao, J., Wang, D., Li, X., Zhang, D., Xu, Q., & Zeng, G. (2018). Effect of diclofenac on the production of volatile fatty acids from anaerobic fermentation of waste activated sludge. Bioresource Technology, 254, 7–15.
Johnson, A. C., Dumont, E., Williams, R. J., Oldenkamp, R., Cisowska, I., & Sumpter, J. P. (2013). Do concentrations of ethinylestradiol, estradiol, and diclofenac in European rivers exceed proposed EU environmental quality standards. Environmental Science & Technology, 47(21), 12297–12304.
Kosjek, T., Heath, E., & Krbavčič, A. (2005). Determination of non-steroidal anti-inflammatory drug (NSAIDs) residues in water samples. Environment International, 31(5), 679–685.
Kunkel, U., & Radke, M. (2011). Reactive tracer test to evaluate the fate of pharmaceuticals in rivers. Environmental Science & Technology, 45(15), 6296–6302.
Kunkel, U., & Radke, M. (2012). Fate of pharmaceuticals in rivers: deriving a benchmark dataset at favorable attenuation conditions. Water Research, 46(17), 5551–5565.
Letzel, M., Metzner, G., & Letzel, T. (2009). Exposure assessment of the pharmaceutical diclofenac based on long-term measurements of the aquatic input. Environment International, 35(2), 363–368.
Lonappan, L., Pulicharla, R., Rouissi, T., Brar, S. K., Verma, M., Surampalli, R. Y., & Valero, J. R. (2016). Diclofenac in municipal wastewater treatment plant: quantification using laser diode thermal desorption—atmospheric pressure chemical ionization—tandem mass spectrometry approach in comparison with an established liquid chromatography-electrospray ionization–tandem mass spectrometry method. Journal of Chromatography A, 1433, 106–113.
Lonappan, L., Brar, S. K., Das, R. K., Verma, M., & Surampalli, R. Y. (2016a). Diclofenac and its transformation products: environmental occurrence and toxicity-a review. Environment International, 96, 127–138.
López-Serna, R., Petrović, M., & Barceló, D. (2012). Occurrence and distribution of multi-class pharmaceuticals and their active metabolites and transformation products in the Ebro River basin (NE Spain). Science of the Total Environment, 440, 280–289.
Ma, R., Wang, B., Lu, S., Zhang, Y., Yin, L., Huang, J., et al. (2016). Characterization of pharmaceutically active compounds in Dongting Lake, China: occurrence, chiral profiling and environmental risk. Science of the Total Environment, 557, 268–275.
Orias, F., & Perrodin, Y. (2013). Characterisation of the ecotoxicity of hospital effluents: a review. Science of the Total Environment, 454, 250–276.
Osorio, V., Imbert-Bouchard, M., Zonja, B., Abad, J. L., Pérez, S., & Barceló, D. (2014). Simultaneous determination of diclofenac, its human metabolites and microbial nitration/nitrosation transformation products in wastewaters by liquid chromatography/quadrupole-linear ion trap mass spectrometry. Journal of Chromatography A, 1347, 63–71.
Prakash, V., Bishwakarma, M. C., Chaudhary, A., Cuthbert, R., Dave, R., Kulkarni, M., et al. (2012). The population decline of Gyps vultures in India and Nepal has slowed since veterinary use of diclofenac was banned. PLoS One, 7(11), e49118.
Qi, W., Singer, H., Berg, M., Müller, B., Pernet-Coudrier, B., Liu, H., & Qu, J. (2015). Elimination of polar micropollutants and anthropogenic markers by wastewater treatment in Beijing, China. Chemosphere, 119, 1054–1061.
Rehman, M. S. U., Rashid, N., Ashfaq, M., Saif, A., Ahmad, N., & Han, J. I. (2015). Global risk of pharmaceutical contamination from highly populated developing countries. Chemosphere, 138, 1045–1055.
Scheurell, M., Franke, S., Shah, R. M., & Hühnerfuss, H. (2009). Occurrence of diclofenac and its metabolites in surface water and effluent samples from Karachi, Pakistan. Chemosphere, 77(6), 870–876.
Schwarz, S., Schmieg, H., Scheurer, M., Köhler, H. R., & Triebskorn, R. (2017). Impact of the NSAID diclofenac on survival, development, behaviour and health of embryonic and juvenile stages of brown trout. Salmo trutta f. fario. Science of The Total Environment, 607, 1026–1036.
Sim, W. J., Lee, J. W., Lee, E. S., Shin, S. K., Hwang, S. R., & Oh, J. E. (2011). Occurrence and distribution of pharmaceuticals in wastewater from households, livestock farms, hospitals and pharmaceutical manufactures. Chemosphere, 82(2), 179–186.
Stülten, D., Zühlke, S., Lamshöft, M., & Spiteller, M. (2008). Occurrence of diclofenac and selected metabolites in sewage effluents. Science of the Total Environment, 405(1–3), 310–316.
Tewari, S., Jindal, R., Kho, Y. L., Eo, S., & Choi, K. (2013). Major pharmaceutical residues in wastewater treatment plants and receiving waters in Bangkok, Thailand, and associated ecological risks. Chemosphere, 91(5), 697–704.
Verlicchi, P., & Zambello, E. (2015). Pharmaceuticals and personal care products in untreated and treated sewage sludge: occurrence and environmental risk in the case of application on soil—a critical review. Science of the Total Environment, 538, 750–767.
Verlicchi, P., Al Aukidy, M., & Zambello, E. (2012). Occurrence of pharmaceutical compounds in urban wastewater: removal, mass load and environmental risk after a secondary treatment—a review. Science of the Total Environment, 429, 123–155.
Vulliet, E., Cren-Olivé, C., & Grenier-Loustalot, M. F. (2011). Occurrence of pharmaceuticals and hormones in drinking water treated from surface waters. Environmental Chemistry Letters, 9(1), 103–114.
Webb, S. F. (2001). A data-based perspective on the environmental risk assessment of human pharmaceuticals I—collation of available ecotoxicity data. In Pharmaceuticals in the Environment (pp. 175–201). Berlin, Heidelberg: Springer.
Wilkinson, J. L., Swinden, J., Hooda, P. S., Barker, J., & Barton, S. (2016). Markers of anthropogenic contamination: a validated method for quantification of pharmaceuticals, illicit drug metabolites, perfluorinated compounds, and plasticisers in sewage treatment effluent and rain runoff. Chemosphere, 159, 638–646.
Yan, Q., Gao, X., Chen, Y. P., Peng, X. Y., Zhang, Y. X., Gan, X. M., et al. (2014). Occurrence, fate and ecotoxicological assessment of pharmaceutically active compounds in wastewater and sludge from wastewater treatment plants in Chongqing, the Three Gorges Reservoir Area. Science of the Total Environment, 470, 618–630.
Yoon, Y., Ryu, J., Oh, J., Choi, B. G., & Snyder, S. A. (2010). Occurrence of endocrine disrupting compounds, pharmaceuticals, and personal care products in the Han River (Seoul, South Korea). Science of the Total Environment, 408(3), 636–643.
Zhang, Y., Geißen, S. U., & Gal, C. (2008). Carbamazepine and diclofenac: removal in wastewater treatment plants and occurrence in water bodies. Chemosphere, 73(8), 1151–1161.
Acknowledgments
The authors wish to express their thanks to Dept. Chemistry, QAU for providing technical expertise and assistance in HPLC analysis.
Funding
The present study was financially supported by the specialized University Research Funds (URF) of Quaid-i-Azam University (QAU), Islamabad.
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Hanif, H., Waseem, A., Kali, S. et al. Environmental risk assessment of diclofenac residues in surface waters and wastewater: a hidden global threat to aquatic ecosystem. Environ Monit Assess 192, 204 (2020). https://doi.org/10.1007/s10661-020-8151-3
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DOI: https://doi.org/10.1007/s10661-020-8151-3