Suchergebnisse

Endocrine active therapeutics such as steroid hormones gain increasing focus in environmental research as it was reported that they cause endocrine disruption in aquatic organisms exposed to environmentally relevant concentrations. Data about occurrence and fate of steroid hormones are scare. In this study occurrence of about 60 steroids in wastewater treatment plant effluents and surface waters as well as the fate and biodegradability of corticosteroids and progestogens in activated sludge treatment were investigated. Corticosteroids and progestogens were prioritized in views of their high prescription and potency to impact endocrine-related functions. A reliable analytical method for the simultaneous determination of mineralocorticoids, glucocorticoids and progestogens in the aquatic environment was developed. Utilizing this method three mineralocorticoids, 23 glucocorticoids and 10 progestogens could be detected in the analyzed samples, many of them were detected for the first time in the environment, particularly in Germany and the EU. Moreover, biodegradation studies were designed to enable the comparison of the biodegradability and transformation processes in activated sludge treatment for structure-related steroids under standardized aerobic conditions. Half-lives ranged from 14 d suggesting large variations in the biodegradability. Transformations products were identified by LC-HRMS and transformation pathways were proposed. Based on these data relationships between structure and stability were elaborated. Several of the newly identified transformation products were persistent and some of them could be detected in wastewater treatment plant effluents and surface waters. Hence, these transformation products should be also included in environmental monitoring.

Since the last decades the increasing detections of pharmaceuticals in the aquatic environment and their risk potential for the aquatic life have become an urgent issue. Even though many pharmaceuticals are at least to some extent removed by sorption and biotransformation during conventional wastewater treatment, a quasi continues emission via wastewater treatment plants result in a so called "pseudo-persistence". Furthermore, metabolites and transformation products (TPs) can show comparable or even higher activities. Therefore, a higher prioritization of pharmaceuticals and their metabolites as well as TPs as environmental pollutants in the European Water Framework Directive and German surface waters regulation (Oberflächengewässerverordnung) would be desirable. Determination of pharmaceuticals in the aquatic environment is focused on the liquid phase. However, only a few standardized methods exist. Indeed, physicochemical parameters of some analytes let accumulation in sediment, suspended particular matter and biota seem to be likely. Hence, these matrices could be interesting alternative matrices for monitoring of pharmaceutical residues in surface waters. The aim of this project was the development, optimization, validation and benchmarking of analytical methods for quantification of selected active pharmaceutical ingredients, their metabolites and TPs in different environmental matrices (water, sediment, suspended particular matter and biota). Using these methods occurrence and distribution of the selected analytes in water, sediment, suspended particular matter and biota samples from different locations were determined. Additionally, samples from the German environmental specimen bank were analyzed to investigate possible time trends in concentrations of pharmaceuticals and to demonstrate the potential of the new methods. Finally, recommendations regarding optimal strategies for determination of pharmaceutical residues with different physicochemical properties in water systems were derived from during this project obtained new insights.

Ziel dieses Vorhabens war die Etablierung eines innovativen Monitoringansatzes für Fisch- und Schwebstoffproben auf Basis von generischen Analysenmethoden. Dazu wurden Extraktions- und Analysenmethoden, die eine große Bandbreite an Analyten erfassen, entwickelt und validiert. An ersten Schwebstoffprobensätzen wurden drei Datenauswertungs-Ansätze für eine retrospektive Betrachtung getestet: i) Datenbank gestützte Suche, ii) Suspect-Screening, iii) Unknown-Screening. Anhand der Ergebnisse und durch einen Abgleich mit vorhandenen Quantifizierungsdaten wurden die Chancen und Limitierungen der Screening-Ansätze kritisch beurteilt. Mit Hilfe der Screening-Ansätze konnten verschiedene Fragestellungen bzgl. Vorkommen und Verteilung sowie Priorisierung von Schadstoffen erfolgreich bearbeitet werden. Es konnte gezeigt werden, dass diese Art der Analysen viel Potential zur Verbesserung der Gewässerüberwachung und Beurteilung der Wirksamkeit von Minderungs- bzw. Verbesserungsmaßnahmen beinhalten. Allerdings zeigten sich Limitierungen bezüglich der Nachweisstärke, so dass das Screening für sehr niedrige Schadstoffkonzentrationen (<1 ng/g) nicht geeignet ist. Vor allem im Fall von Biotaproben zeigten sich auf Grund der komplexen Matrix starke Einschränkungen bezüglich der Anwendbarkeit im niedrigen Konzentrationsbereich. Hier sind Optimierung in Bezug auf die Probenvorbereitung und Datenaufnahme/-auswertung notwendig. Die neu entwickelten Methoden sollen zukünftig zum Aufbau digitaler Probenarchive dienen und so die Identifizierung und Priorisierung neuartiger Schadstoffe in Biotaproben und Schwebstoffen ermöglichen.

Since the last decades the increasing currency of pharmaceuticals in the aquatic environment and their risk potential for the aquatic life has become an urgent issue. The number of pharmaceuticals detectable in the low μg/L range in the environment is rising each day. Against this background the aim of this project was the development, optimization, validation and comparison of analytical methods for quantification of selected pharmaceuticals in different environmental matrices (water, sediment, suspended particular matter and biota). High sensitive LC-MS-MS methods for determination of extreme polar, polar and hormonal pharmaceuticals in water samples were developed and validated. Using these methods occurrence and distribution of the selected pharmaceuticals in water with different waste water content were determined. For analysis of pharmaceuticals in particular matter and biota samples extraction and clean-up procedures were tested, but method development is still in process. Furthermore a monitoring campaign was set up and water samples, suspended particular matter and biota (fish) samples from six different sampling sites were taken.

AbstractRiverbed sediments have been identified as temporary and long-term accumulation sites for microplastic particles (MPs), but the relocation and retention mechanisms in riverbeds still need to be better understood. In this study, we investigated the depth-specific occurrence and distribution (abundance, type, and size) of MPs in river sediments down to a depth of 100 cm, which had not been previously investigated in riverbeds. In four sediment freeze cores taken for the Main River (Germany), MPs (≥ 100 µm) were detected using two complementary analytical approaches (spectroscopy and thermoanalytical) over the entire depth with an average of 21.7 ± 21.4 MP/kg or 31.5 ± 28.0 mg/kg. Three vertical trends for MP abundance could be derived, fairly constant in top layers (0–‍30 cm), a decrease in middle layers (30–60 cm), and a strong increase in deep layers (60–100 cm). The dominant polymer types were polyethylene (PE), polypropylene (PP), and polystyrene (PS). Polyethylene terephthalate (PET) and PP were also found in deep layers, albeit with the youngest age of earliest possible occurrence (EPO age of 1973 and 1954). The fraction of smaller-sized MPs (100–500 µm) increased with depth in shallow layers, but the largest MPs (> 1 mm) were detected in deep layers. Based on these findings, we elucidate the relationship between the depth-specific MP distribution and the prevailing processes of MP retention and sediment dynamics in the riverbed. We propose some implications and offer an initial conceptual approach, suggesting the use of microplastics as a potential environmental process tracer for driving riverbed sediment dynamics.

Dieser Bericht fasst die wesentlichen Arbeiten der Umweltprobenbank des Bundes im Jahr 2021 zusammen. Die Umweltprobenbank des Bundes unterstützt die Umsetzung des Vorsorgeprinzips mit einer wissenschaftlichen Infrastruktur, einer umfassende Datenbasis zur Bestimmung und Bewertung des Ist-Zustandes der Umwelt und einer langfristigen Beobachtung der in der Umwelt stattfindenden chemischen, physikalischen und biologischen Entwicklungsprozesse. Dafür sammeln Fachleute Humanproben ausgewählter Standorte gemeinsam mit ökologisch repräsentativen Umweltproben, archivieren sie bei tiefkalten Temperaturen und führen Untersuchungen auf gesundheits- und umweltrelevante Stoffe durch. Auf diese Weise wird auch eine Kontrolle der Wirksamkeit umweltpolitischer Maßnahmen möglich, beispielsweise bei Beschränkungen der Verwendung von Stoffen.

AbstractWith the nationwide introduction of wastewater treatment the overall water quality improved significantly, but challenges remain, including diffuse pollution, historical sediment contamination and the presence of a multitude of anthropogenic chemical species. The implementation of several EU directives in the twenty-first century led to a stronger focus on improving water and sediment quality and the sustainable management of sediments at river basin scale. Hence, in the last 25 years, not only have the regulatory frameworks significantly changed, but also the scientific backbone of our products, delivered to Germany's federal ministries, practitioners from the German Waterways and Shipping Administration, German federal states and the public. In this respect, approaches such as non-target screening, multi-element analysis, effect-based methods, novel approaches in microplastic and nanoparticle analysis and the benefits from the increase in digitalization and automation are key methods and processes to face future challenges, especially those connected to the global climate crisis.

Dieser Bericht fasst die wesentlichen Arbeiten der Umweltprobenbank des Bundes im Jahr 2020 zusammen. Die Umweltprobenbank des Bundes unterstützt die Umsetzung des Vorsorgeprinzips mit einer wissenschaftlichen Infrastruktur, einer umfassende Datenbasis zur Bestimmung und Bewertung des Ist-Zustandes der Umwelt und einer langfristigen Beobachtung der in der Umwelt stattfindenden chemischen, physikalischen und biologischen Entwicklungsprozesse. Dafür sammeln Fachleute Humanproben ausgewählter Standorte gemeinsam mit ökologisch repräsentativen Umweltproben, archivieren sie bei tiefkalten Temperaturen und führen Untersuchungen auf gesundheits- und umweltrelevante Stoffe durch. Auf diese Weise wird auch eine Kontrolle der Wirksamkeit umweltpolitischer Maßnahmen möglich, beispielsweise bei Beschränkungen der Verwendung von Stoffen.