Dissertation
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Dissertation submitted to the Combined Faculties for the Natural Sciences and for Mathematics of the Ruperto-Carola University of Heidelberg, Germany, for the degree of Doctor of Natural Sciences Presented by: Diploma biologist Jan Wölz Born in: Heidelberg Oral-examination: …………………………… Impact of contaminants on aquatic systems and inundated sites with respect to flood events In vitro biotests, chemical target analysis and fractionation methods Referees: Prof. Dr. Thomas Braunbeck Heidelberg Institute of Zoology, University of Heidelberg Prof. Dr. Heinz Karrasch Geographical Institute, University of Heidelberg Acknowledgment This PhD thesis was very pleasant, since it was not only a product of laboratory work and computing, but also the result of an inspiring and friendly atmosphere with colleagues and friends. Therefore, I would like to thank the workgroup Aquatic Ecology & Toxicology Section at the Heidelberg Institute of Zoology, especially Prof. Dr. Thomas Braunbeck and the workgroup Department of Ecosystem Analysis at the RWTH Aachen University, in particular Prof. Dr. Henner Hollert. Both owe my great thanks for their support, help and supervision of my thesis. Beyond this, I would like to thank Prof. Dr. Henner Hollert and Dipl. biol. Thomas-Benjamin Seiler for the perfect collaboration in our in 2007 established Department of Ecosystem Analysis at the RWTH Aachen University. Furthermore, I would like to thank Prof. Dr. Heinz Karrasch for his deep interest in the research topic of this PhD and for being my second supervisor. Good scientific work is supported by friendly and helpful people. My special thanks go to my dear colleagues at both departments Lisa Bragenheim, Markus Brinkmann, Andrea Gerstner, Katja Großhans, Sebastian Hudjetz, Dr. Steffen Keiter, Dr. Thomas Kosmehl, Eva Lammer, Sibylle Maletz, Paula-Suares Rocha, Hanno Zielke and in particular Marit Ernst and Thomas- Benjamin Seiler. I furthermore like to express my sincere thanks to Ulrike Diehl, Susanne Miller and Kerstin Winkens for their support in the lab. I also like to thank the project partners of the RIMAX-Hot cooperation partners and the BMBF for funding this project and, thus, the majority of my PhD thesis. Beyond, I want to thank, in particular, Dr. Werner Brack, Tobias Schulze and Dr. Urte Lübcke-von Varel (UFZ Helmholtz Centre for Environmental Research, Leipzig) for their collaboration, the possibility for effect-directed analysis and their assistance with chemical analysis. Furthermore, PD Dr. Lothar Erdinger and Dr. Andrew Rastall (Institute of Hygiene and Medical Microbiology, University of Heidelberg) for support with the YES assay. Accordingly, my thanks go to Evelyn Claus and Dr. Georg Reifferscheid (Federal Hydrological Institute, Koblenz) for chemical analysis and provision of the Ames Fluctuation assay. Finally, I am very grateful to my parents for all their encouragement and support of my doctoral thesis. Contents I Contents Abstract………………………………………………………………..……………………….1 Zusammenfassung....…………………………………………………..………………………3 1 Introduction ......................................................................................................................... 5 1.1 Chemicals in the (aquatic) environment and legal handling ................................................... 7 1.1.1 Excursus 1: REACH guideline of the European Union for regulation of chemical ........ 8 1.2 Chemicals related to suspended particulate matter.................................................................. 9 1.2.1 Excursus 2: EU Water Framework Directive (WFD) − Integrated river basin management for Europe ................................................................................................................ 13 1.3 Flood events − Impact on flood plains .................................................................................. 14 1.4 Contaminants in the groundwater and aquifers ..................................................................... 16 1.5 Objectives of the study .......................................................................................................... 17 1.6 References ............................................................................................................................. 20 2 Influence of hydrodynamics on sediment ecotoxicity ...................................................... 29 2.1 Role of sediments in freshwater quality ................................................................................ 31 2.2 Factors affecting mobilization of sediments and (bio-)availability of contaminants ............ 32 2.3 Ecotoxicological methods to assess sediment contamination ............................................... 33 2.4 Combined approaches to investigate the influence of hydrodynamics on sediment ecotoxicity ......................................................................................................................................... 34 2.5 Case Study River Neckar (Germany) .................................................................................... 35 2.5.1 Methods ......................................................................................................................... 36 2.6 Results and Discussion .......................................................................................................... 37 2.7 Case Study Morava Catchment Area (Czech Republic) ....................................................... 39 2.8 Conclusions ........................................................................................................................... 42 2.9 References ............................................................................................................................. 43 3 Changes in toxicity and Ah receptor agonist activity of suspended particulate matter during flood events at the rivers Neckar and Rhine ................................................................. 49 3.1 Abstract ................................................................................................................................. 51 3.2 Introduction ........................................................................................................................... 53 3.3 Materials and methods ........................................................................................................... 55 3.3.1 Suspended particulate matter sampling ......................................................................... 55 3.3.2 Sample extraction .......................................................................................................... 56 3.3.3 Water samples ............................................................................................................... 56 3.3.4 Multilayer fractionation ................................................................................................. 56 3.3.5 PCBs and PCDD/Fs − HRGC-HRMS analysis ............................................................. 57 3.3.6 Neutral Red Retention assay ......................................................................................... 58 3.3.7 DR-CALUX assay ......................................................................................................... 58 3.3.8 GPC.2D assay ................................................................................................................ 59 3.3.9 7-ethoxyresorufin-o-deethylase assay ........................................................................... 59 3.3.10 Bio-TEQ values ............................................................................................................. 60 3.3.11 Chem-TEQ values ......................................................................................................... 60 3.4 Results ................................................................................................................................... 61 3.4.1 Neutral Red retention assay ........................................................................................... 61 Contents II 3.4.2 AhR-mediated activity .................................................................................................. 62 3.4.3 DR-CALUX and GPC.2D assay with SPM .................................................................. 63 3.4.4 Multilayer and carbon on celite fractionation................................................................ 64 3.5 Discussion ............................................................................................................................. 66 3.5.1 Cytotoxic effects of complex samples ........................................................................... 66 3.5.2 Ah receptor agonist activity of water samples............................................................... 67 3.5.3 AhR-mediated activity of SPM ..................................................................................... 68 3.5.4 Modification of pollutant composition .......................................................................... 69 3.5.5 Comparison of AhR-mediated activity .......................................................................... 69 3.5.6 Sources of the remobilized PCDD/PCDF ..................................................................... 70 3.5.7 Relevance of persistent compounds analyzed ............................................................... 72 3.6 Conclusions ........................................................................................................................... 72 3.7