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Atmogenic Pollutants As Reactive Tracers for Identification and Quantification of Important Transport Processes in a Karst Area at the Catchment Scale

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Atmogenic Pollutants As Reactive Tracers for Identification and Quantification of Important Transport Processes in a Karst Area at the Catchment Scale Atmogenic pollutants as reactive tracers for identification and quantification of important transport processes in a karst area at the catchment scale Dissertation zur Erlangung des Grades eines Doktors der Naturwissenschaften der Geowissenschaftlichen Fakultät der Eberhard-Karls-Universität Tübingen vorgelegt von Kerstin Schwarz aus Blaubeuren 2010 Tag der mündlichen Prüfung: 22.01.2010 Dekan: Prof. Dr. Peter Grathwohl 1. Berichterstatter: Prof. Dr. Peter Grathwohl 2. Berichterstatter: Prof. Dr. Johannes Barth Herausgeber: Institut für Geowissenschaften der Universität Tübingen Sigwartstraße 10, D-72076 Tübingen Schriftleitung der Reihe C: Zentrum für Angewandte Geowissenschaften (ZAG) Lehrstuhl für Angewandte Geologie Prof. Dr. Thomas Aigner Prof. Dr. Erwin Appel Prof. Dr. Olaf Cirpka Prof. Dr. Peter Grathwohl Prof. Dr. Stefan Haderlein Prof. Dr. Andreas Kappler Redaktion: Dr. Wolfgang Bott ISSN 0935-4948 (Print) ISSN 1610-4706 (Internet) Für meine Eltern Kurzfassung Die Zielsetzung dieser Arbeit war es herauszuarbeiten, welche Prozesse langfristig für den Verbleib persistenter organischer Verbindungen im Boden und für deren Transport ins Grundwasser im Feldmaßstab relevant sind. Dazu wurden Vertreter aus der Gruppe der polyzyklischen aromatischen Kohlenwasserstoffe (PAK) ausgewählt, die in verhältnismäßig hohen Raten und flächenhaft durch die atmosphärische Deposition in Oberböden eingetragen werden und den verschiedensten Prozessen im Untergrund (Ad-/Desorption, Bioabbau, partikelgetragener Transport, "preferential flow", etc.) unterliegen. Die PAK stellen damit reaktive und im Einzugsgebietsmaßstab räumlich integrierende Tracer dar, die es erlauben, die transportrelevanten Prozesse zu identifizieren und zu quantifizieren. Ein geeignetes Karsteinzugsgebiet (Schwäbische Alb, Blautopf) wurde ausgewählt, in dem eine zuverlässige Eintrags- und Austragsmassenbilanz erstellt werden kann und welches zusätzlich erlaubt, Fragen zur Verletzlichkeit und Gefährdung von Karstgrundwässern zu beantworten. Der Eintrag in das Einzugsgebiet erfolgt über die atmosphärische Deposition, die eine sehr konstante Rate über das gesamte Einzugsgebiet aufweist. Es lassen sich jahreszeitlich bedingte Schwankungen nachweisen, mit höheren Werten im Winterhalbjahr. Böden beinhalten das größte Schadstoffinventar und stellen somit einen wichtigen Faktor dar, um die Speicherung und den Transport von PAK zu quantifizieren. Über das Verteilungsmuster kann ausgesagt werden, dass der Eintrag nahezu ausschließlich über die atmosphärische Deposition erfolgt. Im Sickerwasser, das direkt in den Höhlen, sozusagen in-situ, beprobt wird, werden unter "normalen" Fließbedingungen nur sehr niedrige oder gar keine PAK-Konzentrationen gemessen. Diese geringe Mobilisierung konnte im Elutionsversuch im Labor bestätig werden. Bei Schneeschmelzen steigen die Konzentrationen sprunghaft an und übersteigen zum Teil den Grenzwert für Benz(a)pyren (BaP). Diese Ergebnisse lassen sich in den Untersuchungen im Grundwasser wieder finden. Im Blautopf korreliert die zunehmende PAK-Konzentration mit der zunehmenden Schüttung und der Turbidität. Die Korrelation zeigt, dass der Haupt- transportmechanismus von PAK mit Partikeln verbunden ist. Es konnte nicht gezeigt werden, ob die Partikel direkt von der Oberfläche kommen oder resuspendiert werden. Um die niedrigen Konzentrationen im Wasser messen zu können, wurde ein zeitintegrierendes Messsystem entwickelt. Dieses bewährt sich für die Bestimmung von Hintergrundwerten, kann aber einzelne Ereignisse (z.B. Schneeschmelze), nicht auftrennen und somit muss hierfür die konventionelle Wasserprobennahme eingesetzt werden. Die Eintrags-/Austragsmassenbilanz zeigt, dass 90 % der PAK im System verbleiben. Davon werden mehr als 50 % mit Ereignissen ausgetragen. Die PAK reichern sich in den Oberböden an und werden nicht mit dem Grundwasser aus dem Karstsystem ausgetragen. Um die Vorgänge im Untergrund besser verstehen zu können, wurden zusätzlich stabile Isotopen im Wasser untersucht. Das sich jahreszeitlich verändernde isotopische Signal des Niederschlages konnte weder im Sicker- noch im Grundwasser nachgewiesen werden. Dies zeigt eine vollständige Durchmischung und Speicherung des Sickerwassers in der vadosen Zone an. Abstract The aim of this work was to find out which processes are relevant for the fate and transport of persistent organic pollutants POPs in field scale. Therefore, polycyclic aromatic hydrocarbons (PAHs) were chosen, because they are ubiquitous and have a lateral high input rate via atmospheric deposition. They undergo different processes as ad/-desorption, biodegradation, particle-associated transport and preferential flow. Thus, PAHs are reactive and space integrating tracers, which allow identifying and quantifying transport processes. A suitable karst system (Blautopf Catchment) was chosen, for which a reliable input/output mass balance can be established. Additionally, it is possible to answer questions considering the vulnerability of (karst) groundwater. The input into the catchment happens via atmospheric deposition, which shows a stable deposition rate over the whole catchment. Seasonal fluctuations can be detected with higher values during winter. Soils have the largest storage capacity for contaminants. Thus, they are a main factor to quantify the storage and transport processes of PAHs. The distribution patterns show that the atmospheric deposition is responsible for the input. In the seepage water, which is directly sampled in the caves, there are only low or even no concentrations of PAHs during "normal" flow conditions. This low mobilisation could be verified in the laboratory with leaching tests. During snowmelts the concentrations jumped up and exceeded the limit for benz(a)pyrene BaP in drinking water. These results can also be found in the groundwater. In the Blautopf Spring the increasing concentrations of PAHs correlated with the increasing discharge and the turbidity. This correlation shows that the main transport process is linked with particles. It could not be identified if the particles are from the surface or if they have been resuspended in the system. A time integrating sampler was developed to measure the low concentrations of PAHs in the water. This sampling device is proved for background concentrations. However, it is still necessary to use the conventional water sampling for high flow events, as snowmelts or heavy rain events. The input/output mass balance shows that 90 % of the PAHs remain in the system. Of these more than 50 % can be associated with high flow events. PAHs accumulate in the top soils and do not get transported out of the karst system. To understand the processes in the subsurface stable isotopes were investigated. However, the changing isotope signal of the precipitation could not be detected in the seepage and groundwater. This shows a complete mixing and storage of the seepage water in the vadose zone. Acknowledgements This research was funded with great appreciation by the "Deutsche Forschungsgemeinschaft (DFG)" under grants no. GR 971/20-2. The work was established at the Center for Applied Geoscience (ZAG) at the University of Tübingen. I would like to thank my supervisor Prof. Dr. Peter Grathwohl for his constructive criticism, his inspiring ideas, and for the many hints improving continually the progress of this study. I am very grateful to the laboratory team with whom it was a real pleasure to work together. The atmosphere was friendly, almost familiar, and they always had a helping hand when needed. I want to thank Thomas Wendel, Renate Riehle, Renate Seelig, Bernice Nisch, Annegret Walz and Anne Hartmann-Renz. For the success of this work there are so many people who should be mentioned. I would like to thank the Arbeitsgemeinschaft Blautopf, who provided the logger data from the Blautopf, especially Michael Schopper and Rainer Straub and, furthermore, the Höhlen- und Heimatverein Laichingen e.V. who allowed me to place my samplers in their show cave. Here I would like to acknowledge Wolfgang Ufrecht, who was always interested in my work and gave me a lot of tips and support. Next there are Peter Wiest and his family, as well as Mr. Hiller who gave me the possibility to install my groundwater sampler at the Blautopf and to use the electricity from the water supply (Albwasserversorgung). There are some more, but to make it shorter I will only name them: Patrick Thielsch (providing the weather data), Mr. Ogger (mayor of Heroldstatt), Mr. Huber (Landratsamt Ulm), Mr. Nothum (Landesanstalt für Umwelt, Messungen und Naturschutz Baden-Württemberg, Karlsruhe), Prof. Pfeffer, Mr. Selg (LGRB), Bernd Steinhilber, Heiner Taubald, Richard Frank, Annika Barth and all others. I am also thankful to my colleagues who gave me a lot of support during my PhD research. Namely these are Johannes Barth, Tilman Gocht, Dietmar Steidle, Guohui Wang, David Kuntz, Uli Maier, Christina Eberhard, Sanheng Liu, Peter Ring, Cristina Rebello Postigo, Iris Madlener, and Reiner Henzler. Michaela Blessing deserves a special thank you for her friendship. Most importantly, none of this would have been possible without the love and patience of my family. Without them I could not have accomplished this work. They backed and supported me in every situation, especially my father who was my private "Hi-Wi" and accompanied me in the field. And of course there is also my husband Stefan who was always insightful and gave me the required motivation and time to finish it. I Table of Contents 1 INTRODUCTION .......................................................................................................................................
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