Abstract

Currently, there is uncertainty about emissions of pharmaceuticals into larger closed ecosystems that are at risk such as the Baltic Sea. There is an increasing need for selecting the right strategies on advanced wastewater treatment. This study analysed 35 pharmaceuticals and iodinated X-ray contrast media in effluents from 82 Wastewater Treatment Plants (WWTPs) across Denmark, Estonia, Finland, Germany, Latvia, Lithuania, Poland and Sweden. Measured concentrations from Finland and Denmark were compared to predicted effluent concentrations using different levels of refinement. The concentrations predicted by the Total Residue Approach, as proposed by the European Medicines Agency, correlated with R(2) of 0.18 and 0.031 to measured ones for Denmark and Finland, respectively and the predicted data were significantly higher than the measured ones. These correlations improved substantially to R(2) of 0.72 and 0.74 after adjusting for estimated human excretion rates and further to R(2) = 0.91 and 0.78 with the inclusion of removal rates in WWTPs. Temporal analysis of compound variations in a closely monitored WWTP showed minimal fluctuation over days and weeks for most compounds but revealed weekly shifts in iodinated X-ray contrast media due to emergency-only operations at X-ray clinics during weekends and an abrupt seasonal change for gabapentin. The findings underscore the limitations of current predictive models and findings (...) demonstrate how these methodologies can be refined by incorporating human pharmaceutical excretion/metabolization as well as removal in wastewater treatment plants to more accurately forecast pharmaceutical levels in aquatic environments.

Abstract

The overall aim of the CWPharma project is to reduce the load of active pharmaceutical ingredients (APIs) going into the aquatic environment and especially the Baltic Sea. Municipal wastewater treatment plants (WWTPs) are relevant point sources of APIs, as they treat the wastewater from public households, hospitals and industry of the connected catchment area. However, conventional "state-of-the-art" WWTPs can only remove some APIs, which are either easily biodegradable and/or absorbable to activated sludge, whereas other APIs can pass the WWTP with minor to no reduction. Therefore, reduction of a broad range of APIs can only be achieved by using targeted advanced treatment techniques such as ozonation or powdered and granular activated carbon, respectively, which have already been applied on full-scale for API removal in wastewater treatment in Germany and Switzerland and proven their practical and economical suitability. At the usual applied ozone doses, ozonation of secondary effluent does not mineralize (convert an organic substance into inorganic matter) but transforms organic compounds into smaller and (usually) more biodegradable compounds. Secondary effluent is a complex water matrix consisting of hundreds of different organic substances, and it is not feasible to determine all possible transformation products and oxidation by-products, which might be created by the ozonation process. Thus, utilities and water authorities sometimes struggle with the uncertainties of the ozonation process as they perceive difficulties to judge whether oxidation of the organic matrix is beneficial or if it is creating more problems. As chemical analysis of the water only provides quantitative data for known APIs and transformation products for which chemical standards are available, effect-based ecotoxicological test systems can be used to assess the integrated actual toxicity of the whole water matrix. Based on previous research compiled by Völker et al. (2019), ozonation has a positive impact on several toxicological endpoints. But there are also indications that ozonation can create negative effects for a few toxicological endpoints that can be reduced by a suitable post-treatment. However, only little knowledge is available regarding suitable post-treatments and which ecotoxicological test systems are appropriate to evaluate their impact. In addition, post-treatment options might also have beneficial impacts on water quality parameters, APIs and transformation products. Thus, this report will evaluate different aspects regarding the impact of ozonation and its posttreatment options on (i) water quality parameters, (ii) APIs and transformation products (TPs) and (iii) ecotoxicological effects. The evaluation was conducted at three WWTPs in Linköping (SE), Kalundborg (DK) and Berlin (DE) and different post-treatment options such as moving bed bioreactors (MBBR), deep-bed filters, and a constructed wetland.

Abstract

The overall aim of the "Clear Waters from Pharmaceuticals" (CWPharma) project is to provide guidance on how to reduce the load of active pharmaceutical ingredients (APIs) entering the aquatic environment and especially the Baltic Sea. Even though different methods for reducing the amount of APIs entering the wastewater exist and, thus, "end-of-pipe" measures are also necessary. API usage cannot be completely avoided. Municipal wastewater treatment plants (WWTPs) are relevant point sources of APIs as they treat the wastewater from public households, hospitals, and industry of the connected catchment area. However, conventional "state-of-the-art" WWTPs can only remove APIs that are either easily biodegradable and/or absorbable to activated sludge, whereas others can pass the treatment process with no or only minor reductions. Therefore, reduction of a broad range of APIs can only be achieved by using targeted advanced wastewater treatment (AWT) techniques, such as ozonation or application of powdered and granular activated carbon. All of these technologies for API removal are already used at full-scale WWTPs and have proven their practical and economical suitability. This guideline is meant to provide an overview on how to plan, start, and operate AWT technologies for API elimination. The recommendations are based on the experiences and results from the CWPharma project, but also on the available knowledge from Germany and Switzerland, which is collected and distributed by competence centres such as the German Micropollutants Competence Centre Baden-Württemberg (KomS) Verfahrenstechnik Mikroverunreiniungen and the Swiss Plattform as well as by expert groups from the related water associations. Membrane separation via dense membrane such as nanofiltration (NF) or reverse osmosis (RO) was not considered in this guideline, as both technologies produce a brine with high API concentrations. At coastal WWTPs, this brine might be discharged directly to the sea in order to protect fresh water ecosystems, but this would not reduce the API load to the Baltic Sea. Thus, the brine also requires treatment, which makes this approach less economical in comparison to the other established API removal technologies.

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