Assessment of tetracycline contamination in surface and groundwater resources proximal to animal farming houses in Tehran, Iran
© Javid et al. 2016
Received: 13 May 2015
Accepted: 24 January 2016
Published: 1 February 2016
Antibiotics have been increasingly used for veterinary and medical purposes. The overuse of these compounds for these purposes can pollute the environment, water resources in particular. Tetracycline, among other forms of antibiotics, is one of the most applied antibiotic in aquaculture and veterinary medicine. The present study aimed to tack the traces of tetracycline in the effluents of municipal and hospital wastewater treatment plants, surface and groundwater resources and finally the drinking water provided from these water resources.
The samples were taken from Fasha-Foyeh Dam, wells located at Varamin Plain, and Yaftabad; and also, wastewater samples were collected from the wastewater treatment plant effluents of Emam Khomeini Hospital and a municipal wastewater treatment plant which its effluent is being released to the surface water of the area covered in this work. 24 samples were collected in total during July 2012 to December 2012. The prepared samples were analyzed using high-performance liquid chromatography.
Based on the results, mean tetracycline levels in surface and ground water at nearby of animal farms was found to vary from 5.4 to 8.1 ng L-1. Furthermore, the maximum TC concentration of 9.3 ng L-1 was found to be at Yaft-Abad sampling station. Although tetracycline traces could not be detected in any investigated Hospital WWTP effluents, it was tracked in MWWTP effluent samples, in the concentration range of 280 to 540 ng l−1.
The results showed that the concentration of TC in water resource near the animal farms is higher than the other sampling stations. This is related to the usage of antibiotic for animals. In fact, it caused the contamination of water resources and could contribute to radical changes in the ecology of these regions.
KeywordsTetracycline Groundwater resources Surface water resources Drinking water Animal farms
Antibiotics have been increasingly used for veterinary and medical purposes. The increase in the use of these compounds affects both the environment and human health; in other words, the active forms of the antibiotics are being excreted from the body via urine and/or feces into the environment. Considering this, the overuse of these compounds can pollute the water resources . It should be noted that there are various pathways in which these compounds enter into both surface and groundwater resources, including run-off, leakage from lagoons, leaching of manure applied to fields, and leaching from animal housing areas [Watanabe et al.]. The presence of antibiotics, TC in particular, in water and soil can cause some allergies and toxicity, since these compounds are still active . For instance, excreted antibiotics in the environment affect almost all the bacterial species forcing them to develop a resistance toward these compounds . Based on the reports of previously conducted studies, the residues of various forms of antibiotics have been detected in the samples taken from surface and groundwater resources and also drinking water [4, 5]. Furthermore, the antibiotics have also been found in the samples taken from the effluents of both municipal and hospital wastewater treatment plant [6, 7].
Tetracycline (TC), among other forms of antibiotics, is one of the most applied antibiotics in aquaculture and veterinary medicine . It should be noted that this antibiotic has been applied in livestock and poultry productions more than the aquaculture medicine. In addition, tetracycline is being discharged into the environment, water resources in particular, through wastewater effluent of drug manufacturing companies, disposal of non-consumable compounds and expired drugs containing tetracycline, and also from animal and agricultural wastes [9, 10]. TC has been classified among the antibiotics frequently detected in sewage, domestic wastewaters, surface and groundwater resources, drinking water, and sludge . Considering the increase in the usage of TC and also the inefficiency of most conventional wastewater treatment processes in removing this antibiotic, the surface and ground water resources are now at more risk of being polluted with TC. Furthermore, it should be noted that there is not any regulation for routine sampling and analyzing TC level in the water resources. Previously conducted studies showed that one of the most widely used antibiotic in animals is tetracycline .
In the present work, four samples over 6 months from July 2012 to December 2012 were taken; in total, 24 samples were collected and analyzed in this study. Water samples were taken from tap water, Fasha-Foyeh Dam and also specific wells located at Varamin Plain and Yaftabad. In addition, wastewater samples were collected from the effluents of Emam Khomeini Hospital wastewater treatment plant and a municipal wastewater treatment plant. Figure 1 shows Geographical position of places which the samples were taken.
In this study, two locations were selected to take sample from, namely, Varamin Plain and Yaftabad (i. e. wells nearby animal farming houses) to determine whether TC leached to groundwater resources. In addition, Fasha-Foyeh Dam was selected as surface water resource nearby animal farming houses to assess whether TC has been transported by run-off into the most nearby surface water resource; In other words, the sampling took place at nearby water resources of animal farms which their wastewater effluents are being discharged into the resources. Furthermore, the effluents of municipal and hospital wastewater plants which are being released into the same water resources were considered and analyzed in order to detect TC. The wastewater samples were also taken directly from the effluents of WWTPs to assess the amount of TC released from human sources and compare it with water samples mentioned above. Another spot was also selected (i. e. tap water) to determine whether the drinking water is polluted.
Preparing and analyzing the samples
HPLC gradient program used for determination of TC
Mobile phase A (%)
Mobile phase B (%)
According to a study conducted by Shalaby et al., the strata C18-E cartridge was applied to buffer extract the residue; after sample loading, the cartridge was washed by 10 ml of 5 % methanol mixed in water, and tetracycline was eluted with a mixture of 10 ml of methanol and 0.01 M oxalic acid .
The samples were taken by syringe and filtered through 0.45 μm membrane at pre-selected time intervals; then, the samples were measured using high-performance liquid chromatography (HPLC). HPLC consisted of a Knauer LPG pump, an EZ-chrom HPLC system manager program and a UV detector (k-2500). The UV–detector was set at the maximum absorption wavelength of 365 nm. Aliquots of 100 μL were injected manually using a model SGE injection valve (SGE. Australia). MZ-analysentechnik ODS-3 C18 (4.6 mm × 250 mm) packed with 5 μm spherical particles was used for separation. An Acetonitrile (A) aqueous oxalic acid 0.01 M (B) mixture was used as mobile phase at 300C temperature with a constant flow rate of 1.0 mLmin−1. The used mobile phase are shown in Table 1 .
Results and discussion
Mean concentrations of tetracycline in water resource and wastewater treatment plant effluent
TC concentration (ngL-1)
Yaft-abad – (well)
n = 4
n = 4
n = 4
n = 4
n = 4
n = 4
As mentioned above, the highest concentration of TC was found in the samples taken from ground water resources. Although TC has high affinity to soil compounds, the presence of this antibiotic in the samples even in this range is of high importance. It should be noted that the overuse of these drugs causes them to be found in the water resources due mainly to the saturation of soil capacity; in fact, this phenomenon is known as terracumulation [20, 21]. When the soil becomes saturated with TC, the infiltration of water originated from rain into groundwater resources can carry this antibiotic contributing to the pollution of these resources . Considering the fact that TC is still an active antibiotic when it is bounded to soil particles, the presence of it in groundwater resource is indeed a major problem.
In addition, four samples were taken from tap water to determine whether any concentration of TC is in drinking water. The water treated and distributed among the people of the region we took samples from came from a water treatment plant which uses the water resources (i. e. surface and groundwater) mentioned above. As shown in Table 2, the concentration of TC in these samples was negligible.
This work was aimed to survey the contamination of surface and ground water resources with TC in Tehran, Iran. Based on the results, the water sources studied in this work are contaminated with TC and the presence of other types of antibiotics is also probable. The release of TC from the animal farming areas can be implied to be the main source of groundwater resources pollution with this antibiotic. In addition, the release wastewater effluent from WWTP can be considered as a potential source for the contamination of surface water resource with TC. In fact, the presence of this antibiotic in the environment can cause the mutation of the bacterial species and make them resistant to the antibiotics; and also, negatively affect those who use the water from this resource. In this regard, regular monitoring of the presence of antibiotics mostly used in these areas in order to prevent further damage to the environment. In conclusion, so we recommend more monitoring of the existence of antibiotics residues in water resource near the animal farms.
high-performance liquid chromatography
wastewater treatment plant
municipal wastewater treatment plant
This work is part of a PhD dissertation and supported by Tehran University of Medical Sciences. The authors wish to thank the staff of laboratory of School of Public Health. The second part has been published as “Performance of photocatalytic oxidation of tetracycline in aqueous solution by TiO2 nanofibers”.
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- Xu WH, Zhang G, Zou SC, Li XD, Liu YC. Determination of selected antibiotics in the Victoria Harbour and the Pearl River, South China using ighperformance iquid chromatographyeelectrospray ionization tandem mass spectrometry. Environ Pollut. 2007;145:672–9.View ArticleGoogle Scholar
- Kummerer K. The presence of pharmaceuticals in the environment due to human use - present knowledge and future challenges. J Environ Manage. 2009;90:2354–66.View ArticleGoogle Scholar
- Pena A, Albert-Garcia JR, Silva LJG, Lino CM, Calatayud JM. Photo-induced fluorescence of magnesium derivatives of tetracycline antibiotics in wastewater samples. J Hazard Mater. 2010;179:409–14.View ArticleGoogle Scholar
- Yiruhan, Wang QJ, Mo CH, Li YW, Gao P, Tai YP, et al. Determination of four fluoroquinolone antibiotics in tap water in Guangzhou and Macao. Environ Pollut. 2010;158(7):2350–8.View ArticleGoogle Scholar
- Chee-Sanford J, Aminov R, Krapac I, Garrigues-Jeanjean N, Mackie R. Occurrence and diversity of tetracycline resistance genes in lagoons and groundwater underlying two swine production facilities. Appl Environ Microbiol. 2001;67:1494–1502.View ArticleGoogle Scholar
- Brown KD, Kulis J, Thomson B, Chapman TH, Mawhinney DB. Occurrence of antibiotics in hospital, residential, and dairy effluent, municipal wastewater, and the Rio Grande in New Mexico. Sci Total Environ. 2006;366(2-3):772–83.View ArticleGoogle Scholar
- Homem V, Santos L. Degradation and removal methods of antibiotics from aqueous matrices–a review. J Environ Manage. 2011;92(10):2304–47.View ArticleGoogle Scholar
- Sarmah AK, Meyer MT, Boxall ABA. A global perspective on the use, sales, exposure pathways, occurrence, fate and effects of veterinary antibiotics (VAs) in the environment. Chemosphere. 2006;65:725–59.View ArticleGoogle Scholar
- Boxall AB, Kolpin DW, Halling-Sørensen B, Tolls J. Are veterinary medicines causing environmental risks? J Environ Sci Technol. 2003;37:286A–94.View ArticleGoogle Scholar
- Mompelat S, LeBot B, Thomas O. Occurrence and fate of pharmaceutical products and by-products, from resource to drinking water. Environ Int. 2009;35:803–14.View ArticleGoogle Scholar
- Penghua W, Pow-Seng Y, Lim TT. C–N–S tridoped TiO2 for photocatalytic degradation of tetracycline under visible-light irradiation. Appl Catal Gen. 2011;399:252–61.View ArticleGoogle Scholar
- Nödler K, Licha T, Bester K, Sauter M. Development of a multi-residue analytical method, based on liquid chromatography–tandem mass spectrometry, for the simultaneous determination of 46 micro-contaminants in aqueous samples. J Chromatogr A. 2010;1217:6511–21.View ArticleGoogle Scholar
- Shalaby AR, Salama NA, Abou-Raya SH, Emam WH, Mehaya FM. Validation of HPLC method for determination of tetracycline residues in chicken meat and liver. Food Chem. 2011;124:1660–6.View ArticleGoogle Scholar
- Alder AC, McArdell CS, Golet EM, Ibric S, Molnar E, Nipales NS, et al. Occurrence and fate of flouroquinolone, macrolide, and sulfanamide antibiotics during wastewater treatment and in ambient waters in Switzerland. Symposium Series. Washington: American Chemical Society; 2001. 791, p. 56–69.
- Pedersen J, Yeager M, Suffet I. Xenobiotic organic compounds in runoff from fields irrigated with treated wastewater. J Agric Food Chem. 2003;51:1360–72.View ArticleGoogle Scholar
- Hamscher G, Sczesny S, Ho¨per H, Nau H. Determination of persistent tetracycline residues in soil fertilized with liquid manure by high-performance liquid chromatography with lectrospray ionization tandem mass spectrometry. Anal Chem. 2002;74:1509–18.View ArticleGoogle Scholar
- Samuelsen OB, Torsvik V, Ervik A. Long-range changes in oxytetracycline concentration and bacterial resistance towards oxytetracycline in a fish farm sediment after medication. Sci Total Environ. 1992;114:25–36.View ArticleGoogle Scholar
- Batt AL, Snow DD, Aga DS. Occurrence of sulphonamide antimicrobials in private water wells in Washington County, Idaho, USA. Chemosphere. 2006;64:1963–71.View ArticleGoogle Scholar
- Karthikeyan KG, Meyer T. Occurrence of antibiotics in wastewater treatment facilities in Wisconsin, USA. Sci Total Environ. 2006;361:196–207.View ArticleGoogle Scholar
- Miao XS, Bishay F, Chen M, Metcalfe CD. Occurrence of antimicrobials in the final effluents of wastewater treatment plants in Canada. Environ Sci Technol. 2004;38:3533–41.View ArticleGoogle Scholar
- Rooklidge SJ. Environmental antimicrobial contamination from terraccumulation and diffuse pollution pathways. Sci Total Environ. 2004;325:1–13.View ArticleGoogle Scholar
- Tolls J. Sorption of veterinary pharmaceuticals in soils: a review. Environ Sci Technol. 2001;35:3397–406.View ArticleGoogle Scholar