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New Zealand Coals - a Potential Feedstock for Deep Microbial Life New Zealand coals - A potential feedstock for deep microbial life vorgelegt von Diplom Chemiker Clemens Glombitza aus Berlin Von der Fakultät VI - Planen, Bauen, Umwelt der Technischen Universität Berlin zur Erlangung des akademischen Grades Doktor der Naturwissenschaften Dr. rer. nat. genehmigte Dissertation Promotionsausschuss: Vorsitzender: Prof.Dr. Gerhard Franz Berichter: Prof.Dr. Brian Horsfield Berichter: Prof.Dr. Philippe Schaeffer Tag der wissenschaftlichen Aussprache: 14.12.2010 Berlin 2011 D83 Fakultät VI - Planen, Bauen, Umwelt der Technischen Universität Berlin Author: Clemens Glombitza Umschlaggestaltung: Clemens Gombitza Die Arbeiten im Rahmen dieser Dissertation wurden am Helmholtz Zentrum Potsdam, Deutsches GeoforschungsZentrum (GFZ) in der Sektion 4.3 Organische Geochemie (Prof.Dr. Biran Horsfield) durchgeführt. Diese Dissertation wurde mit LATEX unter Verwendung vom MiKTeX 2.7 und TeXnic Center erstellt. Sie ist ebenfalls als elektronische Version (PDF) über das digitale Repositorium (System OPUS) der Technischen Universität Berlin erhältlich. Webadresse: http://opus.kobv.de/tuberlin Berlin, 2011 There is a theory that states that if anyone ever discovers what the universe is for and why it is here, it will be replaced by something even more bizzare and inexplicable. There is another theory that states this has already happened. D.Adams 1 Statement of original authorship I, Clemens Glombitza, hereby state that the work contained in this thesis has not previously been submitted for assessment, either in whole or in part, by either myself or any other person at either the Fakultät VI - Planen, Bauen, Umwelt at the Technical University of Berlin or at any other institution except where explicitly acknowledged. To the best of my knowledge and belief, the thesis contains no material which has been previously published or written by another person except where due reference is made. Hiermit erkläre ich, Clemens Glombitza, dass diese Arbeit bisher von mir weder an der Fakultät VI - Planen, Bauen, Umwelt der Technischen Universität Berlin noch einer anderen wissenschaftlichen Einrichtung zum Zwecke der Promotion eingereicht wurde. Ferner erkläre ich, dass ich diese Arbeit selbständig verfasst und keine anderen als die darin angegebenen Quellen und Hilfsmittel benutzt habe. , Clemens Glombitza 3 Publications In the scope of this thesis the following articles and conference distributions were published. Articles: Glombitza, C., Mangelsdorf, K., Horsfield, B. (in press). Structural insights from boron tribromide ether cleavage into lignites and low matu- rity coals from the New Zealand Coal Band. Organic Geochemistry, DOI:10.1016/j.orggeochem.2010.12.005. Glombitza, C., Mangelsdorf, K., Horsfield, B. (2009). Maturation related changes in the distribution of ester bound fatty acids and alcohols in a coal series from the New Zealand Coal Band covering diagenetic to cata- genetic coalification levels. Organic Geochemistry, 40(10):1063-1073. Glombitza, C., Mangelsdorf, K., Horsfield, B. (2009). A novel procedure to de- tect low molecular weight compounds released by alkaline ester cleav- age from low maturity coals to assess its feedstock potential for deep microbial life. Organic Geochemistry, 40(2):175-183. Poster presentations on conferences: Glombitza, C., Mangelsdorf, K., Vieth, A., Sykes, R., K., Horsfield, B. (2009). Low mature coals as potential feedstock for deep microbial life. 24th 5 International Meeting on Organic Geochemistry - IMOG (Bremen, Germany, 06.09.-11.09.2009), Book of Abstracts, 103. Glombitza, C., Mangelsdorf, K., Horsfield, B. (2008). Alkaline ester cleavage to examine the feedstock potential of low mature coals for deep microbial populations. European Geosciences Union General Assembly - EGU (Vienna, Austria, 13.04.-18.04.2008), Geophysical Research Abstracts, 10, EGU2008-A-07643. Glombitza, C., Mangelsdorf, K., Horsfield, B. (2007). Investigation of the structural composition of sedimentary organic matter to assess its feed- stock potential for deep microbial populations. 23rd International Meet- ing on Organic Geochemistry - IMOG (Torquay, Devon, United Kingdom, 09.09.-14.09.2007), Book of Abstracts, 439-440. Glombitza, C., Mangelsdorf, K., Horsfield, B. (2006). New Zealand Coals - A potential feedstock for deep microbial population. 2. Annual PhD Meet- ing at Helmholtz Centre Potsdam - German Research Centre for Geo- sciences. 6 Acknowledgements First of all my thanks go out to my supervisor Dr. Kai Mangelsdorf for un- countable inspiring discussions and his excellent supervision, without this, the present work would not have been possible, and to Prof.Dr. Brian Hors- field for providing the themes and topics under investigation and the place in his organic geochemistry group and with this, for giving me the opportunity to receive an insight into this intriguing and challenging scientific discipline. Further, i’d like to thank Prof.Dr. Philippe Schaeffer (CNRS, Strassbourg) and Dr. Jan Schwarzbauer (RWTH, Aachen) for sharing knowledge and pro- viding tips on chemical degradation procedures. The Helmholtz Association is gratefully acknowleged for the financial support of this work. Special thanks go out to the technical staff at the organic geochemistry group at GFZ, namely Cornelia Karger for GC-MS measurements, Kristin Günter for IC measurements and Ferdinand Perssen for pyrolysis GC-MS and pyrolysis GC-FID measurements as well as Anke Kaminsky for support in laboratory work. The guest student Jens Müller is thanked for the good lab work during his internship. I’d like to thank and salute my colleagues and friends Katja Theuerkorn, Alex Vetter and Nick Mahlstedt for sharing all the good and bad times. Furthermore, I’d like to thank all fellows at the OG group for providing a good working atmosphere. Ich danke meiner Familie, die mich immer mit Interesse und Hilfsbe- reitschaft begleitet haben. Mein Dank gilt ebenso meinen Freunden, die mir reichlich Abwechslung verschafft haben und mein Leben stets vielseitig hal- ten. 7 Abstract During the last decades of biogeochemical and microbiological research, the widespread occurrence of microorganisms was demonstrated in deep marine and terrestrial sediments. With this discovery inevitably, the question of potential carbon and energy sources for this deep subsurface microbial life arises. In sedimentary systems, such a source is provided by the buried organic matter deposited over geological times. During geochemical and geothermal maturation, these organic material undergoes biotic and abiotic alteration processes and is suggested, to release potential substrates into the surrounding. Previous studies showed, that especially oxygen containing compounds are lost from the macromolecular matrix during diagenesis and early catagenesis (Putschew et al., 1998; Lis et al., 2005; Petersen et al., 2008). Oxygen containing low molecular weight organic acids (LMWOAs) such as formate, acetate and oxalate represent important substrates for mi- crobial metabolism. Thus, lithologies containing accumulated sedimentary organic matter (e.g. lignites and coals) may provide a large feedstock for deep microbial life releasing LMWOAs into the pore water during maturation. In this thesis, lignite and coal samples from sedimentary basins of New Zealand, covering a broad and almost continuous maturity range from Cre- taceous to Pleistocene age and representing diagenetic to catagenetic coali- fication levels (vitrinite reflection: 0.27% to 0.80%), were investigated to es- timate their feedstock potential for deep microbial life using a novel devel- oped analytical procedure to analyse kerogen-bound LMWOAs liberated by selective chemical degradation reactions. Formate, acetate and oxalate were found to decrease continously from early diagenesis to early catagenesis. 9 This suggests a constant release of these compounds during this maturation interval providing a suitable feedstock for microbial ecosystems in geologi- cal time spans. Investigaton of a transect from organic carbon rich (lignite) into poor lithologies (silt and sandstones) from the DEBITS-1 well, drilled in the Waikato coal area (North Island of New Zealand) suggested that the lignite layers sustain microbial communities inhabiting the adjacent more permeable layers (sandstone) by releasing substrates into the surrounding lithologies (feeder-carrier hypothesis). Investigations of kerogen-bound high molecular weight fatty acids show for the long chain fatty acids (C20-C30) rep- resenting a terrestrial plant material signal a constant decrease during diage- nesis and early catagenesis. In contrast, the short chain fatty acids (mainly C16 and C18) show an increase again during early catagenesis, an interval where the release of hydrocarbons slowly starts but temperatures are still compatible with microbial life. These increasing abundance of C16 and C18 fatty acids (being also main constituents in cell membrane phospholipids of bacteria) might suggest an increased microbial community stimulated by the geothermal release of hydrocarbons (bio-geo coupling hypothesis). Hydrolysis of kerogen-bound LMWOAs is suggested to be the most fa- vorable abiotic process releasing potential substrates into the pore water. Kinetic investigations suggested that the hydrolysis appears to be a rela- tively fast process and, thus, the observed substrate release from lignites and coals over geological times must be influenced and slowed down by further processes such as e.g. pore space, permeability, pore water flow and diffu- sion. The calculated
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