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Source Identification and Specific Degradability of Particulate and Sedimentary Organic Matter in Reservoirs

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Source Identification and Specific Degradability of Particulate and Sedimentary Organic Matter in Reservoirs SOURCE IDENTIFICATION AND SPECIFIC DEGRADABILITY OF PARTICULATE AND SEDIMENTARY ORGANIC MATTER IN RESERVOIRS Dissertation zur Erlangung des Doktorgrades der Naturwissenschaften (Dr. rer. nat.) der Naturwissenschaftlichen Fakultät III, Agrar- und Ernährungswissenschaften, Geowissenschaften und Informatik der Martin-Luther-Universität Halle-Wittenberg vorgelegt von Frau Xiaoqing Liu geb. am 22.Mai 1988 in Jiangxi, China Halle (Saale), den 06.11.2017 Gutachter: Prof. Dr. Kurt Friese Helmholtz-Zentrum für Umweltforschung -UFZ, Department Seenforschung Prof. Dr. Herbert Pöllmann Martin-Luther-Universität Halle-Wittenberg, Institut für Geowissenschaften und Geographie Prof. Dr. Harald Biester Technische Universität Braunschweig, Institut für Geoökologie Tag der Verteidigung: Halle (Saale), 19.03.2018 Sometimes ever, sometimes never... Passion and great idea also… Acknowledgements Acknowledgements The work of this dissertation was carried out from 2014 to 2017 at the Department of Lake Research of Helmholtz Centre for Environmental Research (UFZ) in Magdeburg. First and foremost my deepest gratitude goes to my first supervisor, Prof. Dr. Kurt Friese. Without his research expertise, excellent guidance, vast knowledge, persistent inspiration, continuous optimism concerning my work, this dissertation would not have been possible. He has made any available efforts in a number of ways to give me the best research platform and work atmosphere during these three years. My heartfelt appreciation also goes to my other supervisors, Dr. Karsten Rinke and Dr. Katrin Wendt-Potthoff, for the quick responses to my requests, and for their insightful comments and constructive suggestions to my work. Besides my supervisors, I have to gratefully acknowledge the members of my dissertation committee: Prof. Dr. Kurt Friese, Prof. Dr. Harald Biester and Prof. Dr. Herbert Pöllmann. I thank you for their time and efforts to evaluate this dissertation. The financial support from China Scholarship Council for my stay in Germany is highly appreciated. I would also like to express my gratitude to the graduate school of UFZ-HIGRADE for organizing a wide range of courses and activities, and for funding my participation to conferences and external language training. I want to to thank again Dr. Karsten Rinke, as the head of Department of Lake Research, for supporting me to attend workshops and conferences. I am also deeply grateful to Dr. Barbara Witter (Scientific Coordinator of the Graduate Academy, Otto-von-Guericke-University Magdeburg) who offered me the chances to take the useful courses and meaningful academic activities in the university. All these supports enabled me to gather new ideas, gain further knowledge, and develop soft skills, which greatly contribute to this work. It is a pleasure to thank those who helped me with the experimental work. Special thanks go to Dr. Wolf von Tümpling for the permission to carry out my experiments in the Central Laboratory for Water Analytics & Chemometrics (GEWANA). I would like to gratefully acknowledge Ines Locker from GEWANA for the measurement of stable isotope ratios and Dr. Liane Hilfert from Institute for Chemistry, Otto-von-Guericke-University of Magdeburg for characterizing the structural composition of my samples. I am also particularly grateful for the I Acknowledgements guidance and assistance offered by Michael Herzog, Kerstin Lerche, and other kind technicians in the labs. Wiebke Meyerdierks is heartily thanked for her help during the preparation of samples. Additionally, I sincerely acknowledge the powerful support from the IP group in our institute which largely facilitates my work out of the lab. Discussion with the scientists, Dr. Bertram Boehrer, Dr. Jörg Tittel, Dr. Peter Herzsprung and Dr. Matthias Koschorreck is very instructive and inspirational. The warm encouragement from Dr. Martin Schultze, Burkhard Kuehn and Corinna Völkner will be always kept in my mind. I am indebted to many of my colleagues to back my work and life in Germany in numerous ways. I would like to show my heartful appreciation to Dr. Karoline Morling, Valerie Wentzky, Dr. Marieke Frassl, Dr. Tallent Dadi, Katja Westphal, Claudia Theilmann, Dr. Erik Sartori Gontijo, Gunsmaa Batbayar, Xiaoqiang Yang, Jingshui Huang, Florian Pöhlein, Eva Hasikova, Peiying Lin and the other colleagues for giving immense help and cheerful environment to work in these three years. My time in UFZ is most enjoyable and memorable as it has been a source of joy, passions, good ideas, collaboration and friendships. I owe my deepest gratitude to my parents and sisters. They undertook all the other pressure and responsibilities so that I could concentrate on my work and cheer myself up in difficulty. I also owe a great debt of gratitude to the family of Foerster, from whom I received the warmest care and solicitude in Germany. Last but not least this dissertation would not have come to a successful completion without the encouragement and support from the friends in my homeland. Above all, I cannot imagine how to finish my Ph.D. work without the faithful support from the groups and people I listed above, or those I omitted inadvertently. I have appreciated sincerely and keenly. Thank you. Magdeburg November 2017 II Summary Summary Freshwaters and their sediments contain a substantial amount of allochthonous and autochthonous organic matter (OM). The turnover of this OM pool in the water columns and sediments plays a significant role in the regional and global carbon (C) cycle and in climate change. The mechanisms involved in OM turnover have not been well elucidated as they are controlled by numerous interactive factors exhibiting a high temporal and spatial variability. Moreover, OM in aquatic systems is inherently complex and its constituents have undergone varying degrees of degradation. Knowledge of whether and how these organic components are degraded or preserved is essential to understand the biogeochemistry of OM in aquatic systems. This thesis aimed at 1) identifying the terrestrial and aquatic OM sources in reservoirs, 2) elucidating the degradation of OM in sediments at a biomacromolecular level in different depths. This was carried out at two study sites, Hassel and Rappbode pre-dam, which are part of the Rappbode Reservoir System in Germany. The identification of OM sources in sinking material and buried sediments was accomplished by using biogeochemical proxies, carbon to nitrogen ratio (C/N) as well as carbon and nitrogen stable isotopic compositions (δ13C and δ15N). These proxies were also applied to study the degradation of OM. Processes of the specific degradation of the main organic components (lipids, lignins, proteins and carbohydrates) in sediments were described by quantifying those components through a sequential chemical fractionation procedure. This procedure combined four chemical fractionation methods, yielding a fraction of proteins and carbohydrates and a fraction of lipids and lignins. The new developed stepwise fractionation procedure enabled the determination of C and N contents as well as stable isotopic compositions of OM fractions of different stabilities. Furthermore, it confirmed that δ13C and δ15N can be used for indicating changes of biomacromolecular composition in sedimentary OM. C/N ratio and δ15N recorded effectively the accumulation and degradation of POM in the water column. Comparing C/N ratios and δ15N values of sediment trap material with deposited sediments revealed that the trapped material contained more aquatic OM than the deposited material. The relative aquatic POM contribution to sediment trap material exhibited no evident seasonal trend in the mesotrophic Rappbode pre-dam. By contrast, sediment trap material in the III Summary eutrophic Hassel pre-dam had a larger contribution of aquatic detritus in summer, which corresponded with a higher primary productivity in the water column. Proportions of aquatic and terrestrial OM in sediments showed a large variability among the sampling sites in both pre-dams. Terrestrial OM accounted for 20-70% of total sedimentary OM in both pre-dams. The highest proportion was found in the surface sediments at the shallow site of Rappbode pre-dam, while the lowest proportion was observed at 6-8 cm depth in the sediments of the deep site of Hassel pre-dam. This distribution was mainly caused by a higher aquatic production in the overlying water column as well as a larger amount of microbial biomass in its sediments of the deep site. As revealed by 13C nuclear magnetic resonance analysis, sedimentary OM in Hassel pre-dam was more aliphatic and less aromatic compared to that in Rappbode pre-dam. Within both pre-dams, a higher aromaticity was found at the shallow sites compared to the deep sites. The proportion of terrestrial OM generally increased with sediment depth due to the preferential degradation of aquatic OM. This trend was better observed at the deep sites relative to the shallow sites, because of the larger contribution of aquatic sources to the sediments. The degradation of OM in sediments was caused largely by the decomposition of lipids, proteins and carbohydrates of aquatic origin. It demonstrated that aquatic sedimentary OM was less important as a Carbon sink in a long-term perspective. Moreover, the preferential degradation of 13C-enriched but 15N-depleted proteins and carbohydrates over lipids and lignins was confirmed in this work. Most of the OM degradation took place at the deep sites of both pre-dams, although a minor loss of labile OM was still
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