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.

This report covers the results of the Clear Waters from Pharmaceuticals 2 (CWPharma 21) project continuing the work of the original CWPharma2 project which concluded in December 2020. Both projects were funded by the EU’s Interreg Baltic Sea Region Programme. CWPharma evaluated occurrence and routes of active pharmaceutical ingredients (APIs) in the water cycle and provided recommendations on technical and non-technical measures to reduce API loads entering the Baltic Sea. Recommendations for technical measures were published in the CWPharma ‘Guidelines for advanced API removal processes’ (Stapf et al., 2020), which also includes a modular approach to their successful implementation. The individual modules are: 1) WWTP fitness check, 2) feasibility study, 3) detailed planning, and 4) optimization of existing systems.

Within CWPharma 2, project partners from Denmark, Estonia, Finland, Germany, Latvia, and Poland continued the work of reducing API loads from the aforementioned countries into the Baltic Sea. The focus was to help wastewater treatment plant (WWTP) operators interested in reducing their API discharges to practically implement the four different modules of the guideline. This report summarizes the results of the first module ‘WWTP fitness check’ that have been carried out for about 80 WWTPs from eight Baltic Sea countries and aggregates the anonymized data from the WWTPs to present an overview of general as well as country-specific results, trends and considerations.

Appropriate collection and disposal of medicine-related waste has been identified as one of the main ways to decrease the emission of active pharmaceutical ingredients (APIs) into the environment. Improvement to the take-back and treatment of collected pharmaceutical waste may be considered lowhanging fruit when one is considering measures to reduce API emissions. However, comparable information that would enable estimating the potential impact of these efforts has not been available. Directive 2004/27/EC, related to medicinal products for human use, mandates that EU member states implement appropriate collection schemes for unused or expired human-use medicinal products. However, it does not provide any guidelines on practical implementation of these schemes. Several studies have pointed out significant differences among Member States in this regard. In March 2019, the European Commission published the European Union Strategic Approach to Pharmaceuticals in the Environment. The actions specified therein cover all stages of the pharmaceutical life cycle, from design and production to disposal and waste management. It emphasizes such elements as sharing good practices, co-operating at international level, and improving understanding of the risks. This report is aimed at filling knowledge gaps and proposing good practices for take-back and disposal of unused human and veterinary medicines and other pharmaceutical waste. The report is targeted to e.g. ministries, environment and medicines agencies, supervisory authorities, municipalities, hospitals, NGOs, pharmacists, doctors, and veterinarians. For the report, current national practices for take-back and disposal of unused medicines and other pharmaceutical waste in Denmark, Estonia, Finland, Germany, Latvia, Lithuania, Poland, Russia, and Sweden were evaluated. The pharmaceutical waste originating from households, hospitals and other health care institutions, the pharmaceutical industry, and veterinary use was considered. The proportion of citizens who return unused pharmaceuticals via designated collection points varies greatly between Baltic Sea countries, from about 10% to 70%, with 16–80% disposing of them of as mixed household waste and 3–30% flushing them down the drain. The most commonly cited reason for improper disposal of medicines on households’ part is lack of information about their environmental impacts and how to get rid of them in an environmentally sound manner. Separate collection of unused household pharmaceuticals does not exist in Russia, and the collection mechanism functions poorly in Latvia, Lithuania and Poland. Information on the take-back schemes for unused human medicines is more readily available than is corresponding information on veterinary medicines. We identified, all told, 21 good practices and recommendations for take-back and disposal of unused pharmaceuticals and other pharmaceutical waste and for promoting the rational use of pharmaceuticals in the Baltic Sea region. Nevertheless, implementing them at national level requires particular consideration due to differences in national legislation and other characteristics of the EU Baltic Sea countries and Russia. The good practices identified in this report answer the call issued in the EU strategic approach for an efficient risk-reduction strategy.

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.

Zur Verminderung von Spurenstoffeinträgen in Oberflächengewässer wurden bereits einige Kläranlagen in Deutschland und der Schweiz um eine weitergehende Reinigungsstufe (Ozon oder Aktivkohle) erweitert. Zur Erzielung einer gleichbleibenden Spurenstoffelimination und einer gleichzeitigen Vermeidung von Fehldosierungen (Kosten, Rohstoffeinsatz) werden verlässliche Messverfahren und robuste MSR-Konzepte (Mess-, Regel- und Steuerung) benötigt. Im Rahmen des Projekts „MeReZon" (Schnelle und zuverlässige Messtechnik und Steuer-/Regelkonzepte für eine weitergehende Abwasserreinigung) wurde an einer Pilot-Ozonanlage zur Behandlung von gereinigtem Abwasser untersucht, unter welchen Randbedingungen eine verlässliche Onlinemessung möglich ist. Dabei wurde u.a. die Leistungsfähigkeit eines neu entwickelten Ultraschallreinigungsmoduls zur Vermeidung einer Messwertdrift durch Fouling untersucht und mit den Sonden bzw. Reinigungsmodulen anderer Hersteller in verschiedenen Konfigurationen verglichen. Dabei wurden deutliche Unterschiede festgestellt. Darauf aufbauend wurde das bestehende MSR-Konzept der Ozonanlage optimiert und ein alternierender Messbetrieb, d.h. abwechselnde Beschickung einer Messsonde mit Zu- bzw. Ablauf der Ozonung, implementiert. Die Ergebnisse zeigen, dass mit dem optimierten MSR-Konzept eine stabile Abnahme des SAK254 (SAK254) erzielt werden kann, welche mit der Spurenstoffelimination korreliert. Die erfolgreiche Umsetzung des alternierenden Messbetriebs ermöglicht die Ermittlung der SAK254 Abnahme mit nur einer Messsonde, was prinzipiell Vorteile bei einer Regelung der Ozondosis auf ein stabiles SAK254 mit sich bringt. Zudem konnte gezeigt werden, dass die Onlinemessung der Fluoreszenz eine praktikable Alternative zum SAK254 darstellt, da diese ebenfalls eine Änderung des Ozonbedarfs integral erfassen kann und mit der Spurenstoffelimination korreliert. Die gewonnenen Ergebnisse bieten Messgeräteherstellern wertvolle Anhaltspunkte wie sie ihre Onlinesonden und Reinigungsmodule weiter optimieren können. Das entwickelte MSR-Konzept bzw. der alternierende Messbetrieb kann von Betreibern von Ozonanlagen auf kommunalen Kläranlagen zur Optimierung bestehender oder zukünftiger Anlagen genutzt werden.

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.