Cited by 2,140Pharmaceutical and Antibiotic Environmental ImpactsPesticide Residue Analysis and SafetyAntibiotic Use and Resistance

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Occurrence of antibiotics in the aquatic environment

Hirsch, Roman, Ternes, Thomas, Haberer, Klaus, Kratz, Karl-Ludwig·1999·Science of The Total Environment

DOI 10.1016/s0048-9697(98)00337-4

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Abstract

The recent monitoring of drug residues in the aquatic environment has gained much interest as many pharmaceutical compounds can frequently be found in sewage treatment plant (STP) effluents and river water at concentrations up to several microgram/l. This article describes the analysis of various water samples for 18 antibiotic substances, from the classes of macrolid antibiotics, sulfonamides, penicillins and tetracyclines. Samples were preconcentrated via lyophilization and quantified using HPLC-electrospray-tandem-mass spectrometry. The investigated STP effluents and surface water samples showed frequent appearance of an erythromycin degradation product, roxithromycin and sulfamethoxazole with concentrations up to 6 micrograms/l. Neither tetracyclines nor penicillins could be detected at concentration levels above 50 and 20 ng/l, respectively. From the large number of ground water samples that were taken from agricultural areas in Germany, no contamination by antibiotics was detected except for two sites. This indicates that intake from veterinary applications to the aquatic environment is of minor importance.

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“Hirsch et al. (1999) found that erythromycin could be converted into the dehydrated form in aqueous solutions of less than pH 7.0.”
BackgroundInfluential
Types and quantities of leftover drugs entering the environment via disposal to sewage — Revealed by coroner records
Ruhoy, I. S., & Daughton, C. G. (2007) · The Science of The Total Environment · doi:10.1016/j.scitotenv.2007.08.013 · Cited by 110
“…have provided evidence of the presence of drugs in the aquatic environment (e.g., Fent et al., 2006; Heberer, 2002; Hignite and Azarnoff, 1977; Hirsch et al., 1999), and less frequently in drinking waters (Daughton, in press-b), but the sources and their correlations with disposed quantities…”
Background
Determination of sulfonamides in selected Malaysian swine wastewater by high-performance liquid chromatography
Malintan, N. T., & Mohd, M. A. (2006) · Journal of Chromatography A · doi:10.1016/j.chroma.2006.06.005 · Cited by 109
Multi-residue determination of pharmaceuticals in sludge and sludge enriched soils using pressurized liquid extraction, solid phase extraction and liquid chromatography with tandem mass spectrometry
Barron, L., Tobin, J., & Paull, B. (2008) · Journal of Environmental Monitoring · doi:10.1039/b717453e · Cited by 109
Biological removal of pharmaceuticals and personal care products during laboratory soil aquifer treatment simulation with different primary substrate concentrations.
Onesios, K. M., & Bouwer, E. (2012) · Water Research · doi:10.1016/j.watres.2012.02.001 · Cited by 100
Characterisation of agricultural waste-derived biochars and their sorption potential for sulfamethoxazole in pasture soil: A spectroscopic investigation
Srinivasan, P., & Sarmah, A. K. (2014) · The Science of The Total Environment · doi:10.1016/j.scitotenv.2014.09.048 · Cited by 109
Modified Ponorogo bentonite for the removal of ampicillin from wastewater
Rahardjo, A. K., Susanto, M. J. J., Kurniawan, A., Indraswati, N., & Ismadji, S. (2011) · Journal of Hazardous Materials · doi:10.1016/j.jhazmat.2011.04.052 · Cited by 108
Depletion of chlortetracycline during composting of aged and spiked manures
Bao, Y., Zhou, Q., Guan, L., & Wang, Y. (2008) · Waste Management · doi:10.1016/j.wasman.2008.08.022 · Cited by 107
Potential Changes in Disease Patterns and Pharmaceutical Use in Response to Climate Change
Redshaw, C. H., Stahl-Timmins, W., Fleming, L. E., Davidson, I. M. T., & Depledge, M. H. (2013) · Journal of Toxicology and Environmental Health Part B · doi:10.1080/10937404.2013.802265 · Cited by 108
“This has been illustrated already by the deaths of millions of vultures on the Indian subcontinent following exposure to the nonsteroidal anti-inflammatory drug (NSAID) diclofenac, the well-known (and ongoing) cases of fish feminization associated with excreted components of women’s contraceptive pills, and the global…”
Background
Widespread occurrence and seasonal variation of pharmaceuticals in surface waters and municipal wastewater treatment plants in central Finland
Lindholm‐Lehto, P. C., Ahkola, H. S. J., Knuutinen, J. S., & Herve, S. H. (2016) · Environmental Science and Pollution Research · doi:10.1007/s11356-015-5997-y · Cited by 107
“Consumed pharmaceuticals can be excreted unchanged up to 90 % (Hirsch et al. 1999).”
Background
Degradation of theophylline in a UV254/PS system: Matrix effect and application to a factory effluent
Hakim, S. A., Jaber, S., Eddine, N. Z., Baalbaki, A., & Ghauch, A. (2019) · Chemical Engineering Journal · doi:10.1016/j.cej.2019.122478 · Cited by 107
Analytical techniques in studies of the environmental fate of pharmaceuticals and personal-care products
Kot‐Wasik, A., Dębska, J., & Namieśnik, J. (2006) · TrAC Trends in Analytical Chemistry · doi:10.1016/j.trac.2006.11.004 · Cited by 106
Measles and rubella elimination in the WHO Region for Europe: progress and challenges
O’Connor, P. M., Jankovic, D., Muscat, M., Mamou, M. C. B., Reef, S. E., Papania, M. J., Singh, S., Kaloumenos, T., Butler, R., & Datta, S. S. (2017) · Clinical Microbiology and Infection · doi:10.1016/j.cmi.2017.01.003 · Cited by 123
Toxicological and ecotoxicological risk-based prioritization of pharmaceuticals in the natural environment
Guo, J., Sinclair, C. J., Selby, K., & Boxall, A. B. A. (2016) · Environmental Toxicology and Chemistry · doi:10.1002/etc.3319 · Cited by 105
Spread of antibiotic resistance genes and microbiota in airborne particulate matter, dust, and human airways in the urban hospital
Zhou, Z., Liu, Y., Lin, Z., Shuai, X., Zhu, L., Xu, L., Meng, L.-X., Sun, Y., & Chen, H. (2021) · Environment International · doi:10.1016/j.envint.2021.106501 · Cited by 107
Complete mineralization of the antibiotic amoxicillin by electro-Fenton with a BDD anode
Panizza, M., Dirany, A., Sirés, I., Haidar, M., Oturan, N., & Oturan, M. A. (2014) · Journal of Applied Electrochemistry · doi:10.1007/s10800-014-0740-9 · Cited by 104
“Although their concentration in ground waters tends to be rather low, their effect on aquatic organisms is potentially worrisome because of their bioaccumulative properties, thus causing a long-term exposure that entails unpredictable but irreversible changes such as the growth of microorganisms that are resistant to…”
Background
Biodegradability of 14 C-Labeled Antibiotics in a Modified Laboratory Scale Sewage Treatment Plant at Environmentally Relevant Concentrations
Junker, T., Alexy, R., Knacker, T., & Kümmerer, K. (2005) · Environmental Science & Technology · doi:10.1021/es051321j · Cited by 105
Degradation of chloramphenicol and metronidazole by electro-Fenton process using graphene oxide-Fe3O4 as heterogeneous catalyst
Görmez, F., Görmez, Ö., Gözmen, B., & Kalderis, D. (2019) · Journal of environmental chemical engineering · doi:10.1016/j.jece.2019.102990 · Cited by 103
Critical review of ARGs reduction behavior in various sludge and sewage treatment processes in wastewater treatment plants
Xue, G., Jiang, M., Chen, H., Sun, M. H., Liu, Y., Li, X., & Gao, P. (2019) · Critical Reviews in Environmental Science and Technology · doi:10.1080/10643389.2019.1579629 · Cited by 105
“…frequency and concentration of tetracycline and sulfonamide antibiotics are relatively high in WWTPs, ranging from 0.061 to 1.6 lg/L for tetracycline and 0.009 to 2.8lg/L for sulfonamide in different areas (Batt, Kim, & Aga, 2007; Gao, Shi, et al., 2012; Hirsch et al., 1999; Xu et al., 2015).”
BackgroundInfluential
Occurrence, distribution, and health risk assessment of quinolone antibiotics in water, sediment, and fish species of Qingshitan reservoir, South China
Huang, L., Mo, Y., Wu, Z., Rad, S., Song, X., Zeng, H., Bashir, S., Kang, B., & Chen, Z. (2020) · Scientific Reports · doi:10.1038/s41598-020-72324-9 · Cited by 104
Identification of new transformation products during enzymatic treatment of tetracycline and erythromycin antibiotics at laboratory scale by an on-line turbulent flow liquid-chromatography coupled to a high resolution mass spectrometer LTQ-Orbitrap
Llorca, M., Rodríguez‐Mozaz, S., Couillerot, O., Panigoni, K., de Gunzburg, J., Bayer, S., Czaja, R., & Barceló, ‪. (2014) · Chemosphere · doi:10.1016/j.chemosphere.2014.05.072 · Cited by 104
“…problem is associated to the presence of these 94 compounds into the media since it can induce the development of the so called “environmental 95 antibiotic-resistant pathogens” (Hirsch et al., 1999; Bautitz and Nogueira, 2007; Alighardashi et 96 al., 2009; Khan et al., 2010; Huerta et al., 2013).”
Background
Extraction and preconcentration of salbutamol and terbutaline from aqueous samples using hollow fiber supported liquid membrane containing anionic carrier
Yamini, Y., Reimann, C. T., Vatanara, A., & Jönsson, J. Å. (2006) · Journal of Chromatography A · doi:10.1016/j.chroma.2006.05.001 · Cited by 104
Antibiotic pollution in the Katari subcatchment of the Titicaca Lake: Major transformation products and occurrence of resistance genes
Archundia, D., Duwig, C., Lehembre, F., Chirón, S., Morel, M., Prado, B., Bourdat-Deschamps, M., Vince, E., Avilés, G. P. F., & Martins, J. (2016) · The Science of The Total Environment · doi:10.1016/j.scitotenv.2016.10.129 · Cited by 108
Tetracycline photolysis in natural waters: Loss of antibacterial activity
Wammer, K. H., Slattery, M. T., Stemig, A. M., & Ditty, J. L. (2011) · Chemosphere · doi:10.1016/j.chemosphere.2011.08.051 · Cited by 103
“Given the high usage rates and the fact that 80–90% of tetracycline is excreted unmetabolized (Hirsch et al., 1999), it is not surprising that tetracyclines have been detected in wastewater treatment plant (WWTP) effluents and receiving waters, in addition to waters impacted by agricultural runoff (e.”
Background
Obesity in the United States – Dysbiosis from Exposure to Low-Dose Antibiotics?
Riley, L. W., Raphael, E., & Faerstein, E. (2013) · Frontiers in Public Health · doi:10.3389/fpubh.2013.00069 · Cited by 104
“USA, Spain, Germany (45) Elbe and Saal rivers Erythromycin, sulfamethoxazole, trimethoprim 30–70, 30–70, <30–40 ng/L Germany (46)”
BackgroundInfluential
Acute and chronic effects of erythromycin exposure on oxidative stress and genotoxicity parameters of Oncorhynchus mykiss
Rodrigues, S., Antunes, S. C., Correia, A. T., & Nunes, B. (2016) · The Science of The Total Environment · doi:10.1016/j.scitotenv.2015.10.138 · Cited by 102
“…for the chronic assay are all environmental relevant, being similar or below concentrations of ERY already found in the aquatic environment, near 1 μg/L (Calamari et al., 2003; Ginebreda et al., 2010; Hirsch et al., 1998, 1999) and based on the results obtained for the acute exposure.”
Background
Degradation and intermediates of diclofenac as instructive example for decomposition of recalcitrant pharmaceuticals by hydroxyl radicals generated with pulsed corona plasma in water
Banaschik, R., Jablonowski, H., Bednarski, P. J., & Kolb, J. F. (2017) · Journal of Hazardous Materials · doi:10.1016/j.jhazmat.2017.08.058 · Cited by 105
A multi-biomarker assessment of single and combined effects of norfloxacin and sulfamethoxazole on male goldfish (Carassius auratus)
Liu, J., Lu, G., Wu, D., & Yan, Z. (2014) · Ecotoxicology and Environmental Safety · doi:10.1016/j.ecoenv.2014.01.014 · Cited by 105
Genotoxicity of quinolones: Substituents contribution and transformation products QSAR evaluation using 2D and 3D models
Li, M., Wei, D., Zhao, H., & Du, Y. (2013) · Chemosphere · doi:10.1016/j.chemosphere.2013.09.002 · Cited by 102
“In addition, it was reported that more than 70% of bacteria had become insensitive against at least one antibiotic and exhibited multiple resistance patterns (Hirsch et al., 1999), and the antibiotic resistance of bacteria has become a serious issue.”
Background
Photoproducts of tetracycline and oxytetracycline involving self-sensitized oxidation in aqueous solutions: Effects of Ca2+ and Mg2+
Chen, Y., Li, H., Wang, Z., Tao, T., & Hu, C. (2011) · Journal of Environmental Sciences · doi:10.1016/s1001-0742(10)60625-0 · Cited by 102
Kinetic assessment of the potassium ferrate(VI) oxidation of antibacterial drug sulfamethoxazole
Sharma, V. K., Mishra, S. K., & Ray, A. K. (2005) · Chemosphere · doi:10.1016/j.chemosphere.2005.03.095 · Cited by 102
“Pharmaceuticals are also used as a preventive measure for veterinary purposes and as agricultural herbicides (Hirsch et al., 1999; Battaglin et al., 2000).”
Background
The effectiveness of sewage treatment processes to remove faecal pathogens and antibiotic residues
Hendricks, R., & Pool, E. J. (2012) · Journal of Environmental Science and Health Part A · doi:10.1080/10934529.2012.637432 · Cited by 101
“Additionally, antibiotics are also used in veterinary medicine.[7] In humans and animals, antibiotics exit via urine or faeces.”
Background
Amoxicillin in the Aquatic Environment, Its Fate and Environmental Risk
Elizalde‐Velázquez, A., Gómez‐Oliván, L. M., Galar‐Martínez, M., Islas‐Flores, H., Dublán‐García, O., & SanJuan‐Reyes, N. (2016) · InTech eBooks · doi:10.5772/62049 · Cited by 101
Free-Radical Destruction of β-Lactam Antibiotics in Aqueous Solution
Song, W., Chen, W., Cooper, W. J., Greaves, J., & Miller, G. E. (2008) · The Journal of Physical Chemistry A · doi:10.1021/jp803229a · Cited by 101
Removal efficiency of commonly prescribed antibiotics via tertiary wastewater treatment
Burch, K. D., Han, B., Pichtel, J., & Zubkov, T. S. (2019) · Environmental Science and Pollution Research · doi:10.1007/s11356-019-04170-w · Cited by 100
“…Resources and Environmental Management, Ball State University, Muncie, IN, USA 2 Department of Chemistry, Ball State University, Muncie, IN, USA erythromycin, have been identified in WWTP effluents (Batt et al. 2006; Hirsch et al. 1999;Miao et al. 2004;Watkinson et al. 2007; Yang et al. 2005).”
Background
Determination of antibiotics in aquatic environment by solid-phase extraction followed by liquid chromatography–electrospray ionization mass spectrometry
Rao, R. N., VENKATESWARLU, N. B., & Narsimha, R. (2008) · Journal of Chromatography A · doi:10.1016/j.chroma.2008.02.021 · Cited by 100
Using Central Composite Experimental Design to Optimize the Degradation of Tylosin from Aqueous Solution by Photo-Fenton Reaction
Sarrai, A. E., Hanini, S., Merzouk, N. K., Tassalit, D., Szabó, T., Hernádi, K., & Nagy, L. (2016) · Materials · doi:10.3390/ma9060428 · Cited by 99
“During the last two decades, an increasing interest has been shown in the ecological effects of pharmaceuticals and personal care products, which are released into the environment every year [1,2].”
Background
ISO 14040: Life Cycle Assessment (LCA) – Principles and Guidelines
Arvanitoyannis, I. S. (2008) · Elsevier eBooks · doi:10.1016/b978-012373654-3.50006-7 · Cited by 99
Synthesis and application of CdS nanorods for LED-based photocatalytic degradation of tetracycline antibiotic
Das, S. C., & Ahn, Y. (2021) · Chemosphere · doi:10.1016/j.chemosphere.2021.132870 · Cited by 99

Authors: Hirsch, R., Ternes, T., Haberer, K., & Kratz, K.-L.
Affiliations: Johannes Gutenberg University Mainz (DE)
ORCID: Ternes, Thomas
Kratz, Karl-Ludwig
Venue: Science of The Total Environment
Publisher: Elsevier BV
Published: 1999-01
Volume: 225
Issue: 1-2
Pages: 109-118
ISSN: 0048-9697 (ISSN-L)
DOI: 10.1016/s0048-9697(98)00337-4
OpenAlex: W2029593210
Cited by: 2,140
References: 32
Citations by year: 2026: 19 · 2025: 37 · 2024: 48 · 2023: 54 · 2022: 74 · 2021: 83 · 2020: 100 · 2019: 93 · 2018: 117 · 2017: 103 · 2016: 102 · 2015: 112 · 2014: 121 · 2013: 113 · 2012: 124
FWCI: 25.17
Type: journal article
Language: en
Open access: closed
Licence: www.elsevier.com/tdm/userlicense/1.0/ (tdm)
Locations: The Science of The Total Environment (publishedVersion)
PubMed (publishedVersion)
Funders: Bundesministerium für Bildung und Forschung
Ministry of Environment
Topics: Physical Sciences › Environmental Science › Pollution › Pharmaceutical and Antibiotic Environmental Impacts
Life Sciences › Agricultural and Biological Sciences › Food Science › Pesticide Residue Analysis and Safety
Health Sciences › Medicine › Infectious Diseases › Antibiotic Use and Resistance
Keywords: antibiotic residues, aquatic environment, sewage treatment plant effluent, surface water, groundwater contamination, sulfonamides, penicillin, tetracycline, roxithromycin, sulfamethoxazole, veterinary antibiotic use, agricultural land
MeSH terms: Agriculture, Animals, Anti-Bacterial Agents, Bacteria, Biodegradation, Environmental, Drug Resistance, Microbial, Erythromycin, Germany, Humans, Sewage, Water Pollutants, Chemical

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