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Pharmaceutical residues are widespread in Baltic Sea coastal and offshore waters – Screening for pharmaceuticals and modelling of environmental concentrations of carbamazepine
KTH, School of Engineering Sciences in Chemistry, Biotechnology and Health (CBH), Industrial Biotechnology.
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2018 (English)In: Science of the Total Environment, ISSN 0048-9697, E-ISSN 1879-1026, Vol. 633, p. 1496-1509Article in journal (Refereed) Published
Abstract [en]

The consumption of pharmaceuticals worldwide coupled with modest removal efficiencies of sewage treatment plants have resulted in the presence of pharmaceuticals in aquatic systems globally. In this study, we investigated the environmental concentrations of a selection of 93 pharmaceuticals in 43 locations in the Baltic Sea and Skagerrak. The Baltic Sea is vulnerable to anthropogenic activities due to a long turnover time and a sensitive ecosystem in the brackish water. Thirty-nine of 93 pharmaceuticals were detected in at least one sample, with concentrations ranging between 0.01 and 80 ng/L. One of the pharmaceuticals investigated, the anti-epileptic drug carbamazepine, was widespread in coastal and offshore seawaters (present in 37 of 43 samples). In order to predict concentrations of pharmaceuticals in the sub-basins of the Baltic Sea, a mass balance-based grey box model was set up and the persistent, widely used carbamazepine was selected as the model substance. The model was based on hydrological and meteorological sub-basin characteristics, removal data from smaller watersheds and wastewater treatment plants, and statistics relating to population, consumption and excretion rate of carbamazepine in humans. The grey box model predicted average environmental concentrations of carbamazepine in sub-basins with no significant difference from the measured concentrations, amounting to 0.57-3.2 ng/L depending on sub-basin location. In the Baltic Sea, the removal rate of carbamazepine in seawater was estimated to be 6.2 10(-9) s(-1) based on a calculated half-life time of 3.5 years at 10 degrees C, which demonstrates the long response time of the environment to measures phasing out persistent or slowly degradable substances such as carbamazepine. Sampling, analysis and grey box modelling were all valuable in describing the presence and removal of carbamazepine in the Baltic Sea.

Place, publisher, year, edition, pages
Elsevier, 2018. Vol. 633, p. 1496-1509
Keywords [en]
Baltic Sea, Carbamazepine, Coastal and offshore waters, Half-life time, Model, Pharmaceuticals
National Category
Environmental Sciences
Identifiers
URN: urn:nbn:se:kth:diva-227511DOI: 10.1016/j.scitotenv.2018.03.276ISI: 000432475300145PubMedID: 29758901Scopus ID: 2-s2.0-85044791102OAI: oai:DiVA.org:kth-227511DiVA, id: diva2:1206217
Funder
Mistra - The Swedish Foundation for Strategic Environmental Research
Note

QC 20180516

Available from: 2018-05-16 Created: 2018-05-16 Last updated: 2018-11-26Bibliographically approved
In thesis
1. Pharmaceuticals – improved removal from municipal wastewater and their occurrence in the Baltic Sea
Open this publication in new window or tab >>Pharmaceuticals – improved removal from municipal wastewater and their occurrence in the Baltic Sea
2018 (English)Doctoral thesis, comprehensive summary (Other academic)
Abstract [en]

Pharmaceutical residues are found in the environment due to extensive use in human and veterinary medicine. The active pharmaceutical ingredients (APIs) have a potential impact in non-target organisms. Municipal wastewater treatment plants (WWTPs) are not designed to remove APIs.

In this thesis, two related matters are addressed 1) evaluation of advanced treatment to remove APIs from municipal wastewater and 2) the prevalence and degradation of APIs in the Baltic Sea.

A stationary pilot plant with nanofiltration (NF) and a mobile pilot plant with activated carbon and ozonation were designed to study the removal of APIs at four WWTPs. By NF, removal reached 90%, but the retentate needed further treatment. A predictive model of the rejection of APIs by NF was developed based on the variables: polarizability, globularity, ratio hydrophobic to polar water accessible surface and charge. The pilot plants with granular and powdered activated carbon (GAC) and (PAC) removed more than 95% of the APIs. Screening of activated carbon products was essential, because of a broad variation in adsorption capacity. Recirculation of PAC or longer contact time, increased the removal of APIs. Ozonation with 5-7 g/m3 ozone resulted in 87-95% removal of APIs. Elevated activity and transcription of biomarkers indicated presence of xenobiotics in regular effluent. Chemical analysis of APIs, together with analysis of biomarkers, were valuable and showed that GAC-filtration and ozonation can be implemented to remove APIs in WWTPs, with decreased biomarker responses.

Sampling of the Baltic Sea showed presence of APIs in 41 out of 43 locations. A developed grey box model predicted concentration and half-life of carbamazepine in the Baltic Sea to be 1.8 ng/L and 1300 d respectively.

In conclusion, APIs were removed to 95% by GAC or PAC treatment. The additional treatment resulted in lower biomarker responses than today and some APIs were shown to be widespread in the aquatic environment.

Place, publisher, year, edition, pages
Stockholm: KTH Royal Institute of Technology, 2018. p. 150
Series
TRITA-CBH-FOU ; 2018-62
Keywords
Advanced wastewater treatment, WWTP, pilot plant, pharmaceutical residues, removal of pharmaceuticals, activated carbon, ozonation, nanofiltration, biomarker, Baltic Sea
National Category
Bioprocess Technology
Research subject
Biotechnology
Identifiers
urn:nbn:se:kth:diva-239307 (URN)978-91-7873-047-6 (ISBN)
Public defence
2018-12-20, F3, Lindstedtsvägen 26, Stockholm, 10:00 (English)
Opponent
Supervisors
Funder
Mistra - The Swedish Foundation for Strategic Environmental Research, MistraPharma
Note

QC 20181120

Available from: 2018-11-20 Created: 2018-11-20 Last updated: 2018-11-20Bibliographically approved

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