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The Example of the Hetao Basin

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The Example of the Hetao Basin Arsenic mobilization processes in inland sediment basins – the example of the Hetao Basin Zur Erlangung des akademischen Grades einer DOKTORIN DER NATURWISSENSCHAFTEN (Dr. rer. nat.) von der KIT-Fakultät für Bauingenieur-, Geo- und Umweltwissenschaften des Karlsruher Instituts für Technologie (KIT) genehmigte DISSERTATION von Dipl.-Geoökol. Hongyan Wang aus Shandong, China Tag der mündlichen Prüfung: 19.02.2021 Referent: Prof. Dr. Stefan Norra Korreferent: Prof. Dr. HM. Guo Prof. Dr. Thomas Neumann Karlsruhe, den 19.02.2021 Erklärung Hiermit erkläre ich, dass ich die vorliegende Dissertation, abgesehen von der Benutzung der angegebenen Hilfsmittel, selbständig verfasst habe. Alle Stellen, die gemäß Wortlaut oder Inhalt aus anderen Arbeiten entnommen sind, wurden durch Angabe der Quelle als Entlehnungen kenntlich gemacht. Diese Dissertation liegt in gleicher oder ähnlicher Form keiner anderen Prüfungsbehörde vor. Karlsruhe, im März 2021 Hongyan Wang Acknowledgements Acknowledgements This work could not be completed without the help of the following people: First and sincerely, I express my deepest gratitude to my supervisor – Prof. Dr. Stefan Norra. Thanks Stefan for taking care of my work and life in Germany. In the life, you always tell me relax and enjoy. In the work, you teach me be patient and precise for what I am doing. The scientific freedom you gave to me enables me to find collaborations and to learn to become an independent scientist. Thanks for the encouragement and tolerance for my PhD! I could not have reached those achievements without you, Stefan! Thanks for the countless greetings during my “dark time”, I feel warm with your care staying in Germany. I would like to thank my co-referees Prof. Dr. Huaming Guo and Prof. Dr. Thomas Neumann. Thanks to Professor Guo for providing me opportunities to learn in his group even before I started my PhD, and gave me the chance to accompany him during his field trips. I started my PhD in his group and learned the fundamentals of research. Thanks to him for providing me samples and so much useful information. His diligence and rigours scholarship inspired me to go forward. Thanks also for the sincere suggestions from Professor Neumann, which let my thesis go smoothly and faster. Thank the Chinese Scholarship Council (CSC) for giving me a scholarship to study at the Karlsruhe Institute of Technique (KIT), Germany. It is a wonderful and worthful experience to study in Karlsruhe. I never dreamed I could go abroad before I got this scholarship. Further, I like to express my gratitude to Graduate School for Climate and Environment (GRACE) for giving me funding to do experiments outside, and to travel abroad for conferences. Those experiences increased my networks and broadend my horizons. It is helpful for my future career. My deep and special thanks to Dr. Jörg Göttlicher and Dr. Ralph Steininger. Thank for collecting so many beam times for me and for so many discussions on my experimental details. You taught me a lot of professional knowledge about XAS, and contributed so much to my thesis. Thank you giving me the chance to get closed to such an advanced instrument. I Acknowledgements The warm thanks to Dr. Elisabeth Eiche. You gave me constant help for the laboratory work, I could not have survived in the lab without you. Thank you for so many suggestions for my PhD work, and for sharing your experience with me and therein I was able to finish experiment in short time. I am also grateful for your help during applying beam times in SSRL and ALS even though it was not successful. Thanks, Eli! Thanks as well for Professor Andreas Kappler. You are the first professor to open the collaboration doors to me. I feel so happy and honourable to know and discuss with a professor who has such passion and love for science. You also gave me confidence to look for further collaborators. Thank the funding for collecting Mössbauer spectra for my samples. Thank Dr. James Byrne for countless discussions and numerous simulations for my data. I never met a scientist who is responsible for his/her work like you! I would like to express my gratitude to Professor Liane Benning. You gave me the chance to do SEM and TEM measurements, also discussed my data and manuscript in depth. Your enthusiasm to science encourages me to do science forever! Thank Dr. Jeffrey Perez, you helped me to collect synchrotron and TEM data even without sleep. You always gave me constructive suggestions for my experiments, and always comfort me when my experiments failed. I am happy to meet a friend and collaborator like you! Thank Dr. Heidi Höfer providing me funding and support for EPMA analysis. The “old EPMA instrument” helped me a lot to interpret my data! Thank Professor Agnes Kontny for offering me the chance to measure the magnetic susceptibility, which enabled me to know the exciting minerals! I would like to express my deep gratitude to Ms. Chantalle Kotschenreuther. You can always find something “missed” in the lab. You did not only give help in the lab, but also much more like my sister, gave me help in my life, comfort me when I felt depressed. Thanks, Chantalle! Here, I also thank to all technicians in AGW, Claudia Möβner, Gesine Preuβ, Ralf Wachter, Kristian Nikoloski. Thank you help me analyse countless samples and tolerant my disturbations. I want to thank Flavia and JingWei and Jia. Thank you always to give me an ear and to listen my complains. Without those ladies, I would not have been so happy to spend the PhD time. Special thanks to Nico. Thank you always try to give solutions for difficulties I met in the experiments. II Acknowledgements Thanks, Andrew! Thanks for your help for collecting XAS data. Thank you for the happiness you brought to us. I also want to give thanks to Andre, Andreas, Xiaohui, Jonas, Van. Thank you all to share stories and happy lunch time with me! Thank my friend Yujie, Gai, and Ningyi, thank your company! Thanks to my family! Words cannot express gratitude to parents. You always gave me support and encouragement. Without you I would not have been able to experience this day . Thank my parents in law, thanks for the help to take care of my child. Special thanks to my husband. Thank you always cheering me up in every dark moment. I could not be a PhD student and study abroad without your support. Thank my lovely child, you give me courage to pursue my future. Here, I dedicate this thesis to all my family members. Hongyan Wang 王红岩 Karlsruhe III Abstract Abstract Geogenic groundwater arsenic (As) pollution is a worldwide concern that mainly occurs in south and south-east of Asia, including the Ganges-Brahmaputra-Meghna (GBM) plain, the Red River delta and the Mekong delta as well as basins draining the Yellow River and the Yangtze River. In contrast with flood plains in south and southeast of Asia, inland sediment basins show different depositional environment and chemical groundwater compositions, especially regarding 2- high SO4 concentrations and pH values. Thus, the mechanisms of As release and transport in the aquifers might be different. However, most of the study focusses on those flood plains based on collecting groundwater and sediment samples. In the north of China, the Hetao Basin is a typical inland basin with As concentrations up to 570 µg/L. Here, the As mobilization is complexed by Fe-S-organic carbon coupled interactions. It provides us a natural laboratory to study the As mobilization in the inland basins. In this dissertation, I mainly used high-resolution spectroscopy (e.g. XAS and Mössbauer) and microscopy in combination with other geochemical techniques to interpret the Fe–S–As coupled redox profiles in the sediments under depositional frames of the Hetao Basin. Specifically, 2- the objectives of this study were to 1) trace the depositional environment and source of SO4 in the Holocene–late Pleistocene aquifers sediments, 2) characterize the Fe-As–S coupled redox minerals in the sediment profiles, 3) indicate the influence of Fe-As-S interaction for groundwater As mobilization and 4) elucidate the impact of organic carbon-rich sediments (peats) for As transport. Sediments in the Hetao Basin are probably resourced from the Lang Mountains, as indicated by their similar rare earth element (REE) compositions. Weathering of As-enriched minerals from the Lang Mountains may have contributed to the relatively higher sediment As content (11 mg/kg in average) compared to other sediments from south and southeast of Asia. Carbon isotope (δ13C) of organic carbon in combination with C/N ratio revealed that sediments were mainly deposited in the aquatic environment and corresponded to the fluvial-lacustrine deposit, while the sediments at depths of 10-30 m have mostly lacustrine deposit. The lacustrine depositional environment in the Hetao Basin enables evaporites precipitation. 2- Dissolution of sulfates contributes to the high groundwater SO4 concentration. The Fe-S-organic carbon coupled reactions following by sulfates dissolution under redox oscillations further influences the As partitions in the aquifers. Modelling results suggest that thio-As species, IV Abstract especially thio-arsenate existed in the groundwater and increased As mobilization potentials, while pyrite might form with saturation of FeS2 and incorporated As into its structure. Spectroscopy methods in combination with microscopy, and other geochemical techniques were used to further elucidate the As, S and Fe speciation in the sediments. The As K-edge X-ray absorption near-edge structure spectroscopy (XANES) showed the surface sediments are dominated by As(V) species (84%), and a decreasing trend with depth (R2 = 0.59) was revealed. Iron oxides were predominantly goethite and hematite, which also decreased in concentration with depth as indicated by Fe K-edge extended X-ray absorption fine structure (EXAFS).
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