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Proquest Dissertations Assessing the Carbon Dynamics in Natural and Human-Perturbed Boreal Aquatic Systems Alexandre Ouellet A Thesis in the Department of Chemistry and Biochemistry Presented in Partial Fulfillment of the Requirements For the Degree of Doctor of Philosophy at Concordia University Montreal, Quebec, Canada July 20 10 © Alexandre Ouellet, 2010 Library and Archives Bibliothèque et ?F? Canada Archives Canada Published Heritage Direction du Branch Patrimoine de l'édition 395 Wellington Street 395, rue Wellington Ottawa ON K1A 0N4 Ottawa ON K1A 0N4 Canada Canada Your file Votre référence ISBN: 978-0-494-71129-3 Our file Notre référence ISBN: 978-0-494-71129-3 NOTICE: AVIS: The author has granted a non- L'auteur a accordé une licence non exclusive exclusive license allowing Library and permettant à la Bibliothèque et Archives Archives Canada to reproduce, Canada de reproduire, publier, archiver, publish, archive, preserve, conserve, sauvegarder, conserver, transmettre au public communicate to the public by par télécommunication ou par l'Internet, prêter, telecommunication or on the Internet, distribuer et vendre des thèses partout dans le loan, distribute and sell theses monde, à des fins commerciales ou autres, sur worldwide, for commercial or non- support microforme, papier, électronique et/ou commercial purposes, in microform, autres formats. paper, electronic and/or any other formats. The author retains copyright L'auteur conserve la propriété du droit d'auteur ownership and moral rights in this et des droits moraux qui protège cette thèse. Ni thesis. Neither the thesis nor la thèse ni des extraits substantiels de celle-ci substantial extracts from it may be ne doivent être imprimés ou autrement printed or otherwise reproduced reproduits sans son autorisation. without the author's permission. In compliance with the Canadian Conformément à la loi canadienne sur la Privacy Act some supporting forms protection de la vie privée, quelques may have been removed from this formulaires secondaires ont été enlevés de thesis. cette thèse. While these forms may be included Bien que ces formulaires aient inclus dans in the document page count, their la pagination, il n'y aura aucun contenu removal does not represent any loss manquant. of content from the thesis. ¦+¦ Canada Abstract Assessing the Carbon Dynamics in Natural and Human-Perturbed Boreal Aquatic Systems Alexandre Ouellet, Ph.D. Concordia University, 2010 Most lakes and reservoirs worldwide are supersaturated with respect to water concentrations of carbon dioxide (CO2) and methane (CH4), two potent greenhouse gases (GHG). Although surface water GHG concentrations have been measured for more than three decades in lakes and reservoirs around the globe, the mechanisms leading to GHG supersaturation are still obscure, with the relative contributions of the different GHG producing processes hotly debated. In this study, we evaluated the terrestrial organic matter (OM) exports from land to aquatic systems, followed by its degradation and contribution to the surface freshwaters GHG concentrations. Natural lakes, reservoirs as well as lakes and reservoirs with a wood harvested watershed were sampled in the summer of 2007 and analyzed for a broad variety of bulk water chemical parameters and OM molecular proxies. In order to collect sufficient quantities of OM for the amino acid (AA) and lipid molecular analyses, a tangential flow filtration reverse osmosis systems (TFF-RO) was used following the evaluation of its performance for total OM possible molecular fractionation and recoveries using FTIR, stable carbon isotope signatures (O13C) and total organic carbon (TOC) concentrations. No significant sample fractionation or carry over was obtained with recoveries ranging between 94.6 and 1 06.9 % using the TFF-RO system. All lakes and reservoirs sampled in this study were supersaturated in CO2 and CH4, with wood harvested water bodies and the reservoir having significantly higher water surface iii CO2 concentrations and emissions to the atmosphere compared to the natural lakes. The bulk water and OM chemical and isotopie analyses showed that the increase in terrestrial dissolved organic carbon and total nitrogen concentrations positively influenced bacterial OM degradation, which drove CO2 production. Molecular analyses showed a direct relationship between the increases in bacterial biomarker abundances in the dissolved and sedimentary OM fractions, and higher water CO2 concentrations. This result suggests that OM bacterial oxidation is the most important process leading to GHG production in freshwater aquatic systems. IV Acknowledgements This project was proposed and initiated by a multidisciplinary team; Marc Michel Lucotte, Yves Gélinas, Changhui Peng and Éric Duchemin are kindly acknowledged for their efforts in designing this project. Nicolas Soumis, a research manager working with M. M. Lucotte, is thanked for his help in coordinating and organizing seasonal field campaigns as well as for compiling a huge amount of data in a standardized database. Haibin Wu is acknowledge for his discussions and inputs as for modeling and coupling terrestrial and aquatic systems. I am especially grateful to Jean-Baptiste Plouhinec, a close UQAM collaborator and partner in leading all seven sampling missions; he became my friend as well as a very good and diversified environmental scientist; I admire his work and contributions to the field ofphoto- oxidation. I am thankful to anonymous reviewers of the already published Chapter (2) but also to Robert Panetta, Karine Lalonde, Mina Ibrahim and Denis Brion for helpful discussions and constructive comments on the research design and manuscripts. We extend our thanks to B. Ghaleb (GEOTOP), V. P. Nguyen and L.-H. Bourgoin (Université de Moncton), as well as A. Tessier (CBAMS - Concordia) and Jean- François Hélie for their help with the 10Pb, amino acid, Fe and dissolved inorganic carbon isotopie analyses, respectively. This study was funded through grants (YG and MML) and scholarships (AO and JBP) from BIOCAP-Canada, FQRNT and NSERC, as well as a grant from the Canadian Foundation for Innovation (YG) and GEOTOP. Unrelated to this research, there are key personalities that need to be thanked for daily support; my so loved wife and my son are both acknowledged for their respective positivism and time sacrifice during the last years of this doctorate. My parents always believed in and supported me during all six years of my graduate studies. It is also worth mentioning that Yves Gélinas is one of the best research supervisors that a graduate student can dream of, he always inspired me. Yves equally had good intuitions, great suggestions and truthful criticisms during the realization ofthis project. Thank you Yves, these last six years were terrific. Vl Table of content List ofFigures X1 List ofTables x« Glossary and Definitions xiv 1 The study of aquatic freshwater ecosystems 1 1.1 The carbon cycle in freshwater ecosystems 1 1.2 Greenhouse gases supersaturation in lakes 5 1.3 Anthropogenic effects on GHG fluxes 7 1.3.1 Hydro-electric reservoirs 8 1 .3.2 Wood harvesting activities 1 1 1.4 Organic matter source studies 12 1.4.1 An elemental and isotopie approach 13 1.4.2 A biomarker approach 17 1.5 Thesis format, connecting text and co-author contributions 19 2 Elemental, isotopie and spectroscopic assessment of chemical fractionation of dissolved organic matter sampled with a portable reverse osmosis system 22 2.1 Abstract 23 2.2 Introduction 24 2.3 Materials and Methods 27 2.3.1 Field sampling 27 2.3.2 Microfiltration-Reverse Osmosis (MF-RO) unit 27 2.3.3 TOC measurement 28 2.3.4 EA-IRMS measurements 29 2.3.5 FTIR measurements 29 2.4 Results and discussion 29 2.4.1 Carbon mass balance 30 2.4.2 Sample fractionation 34 vii 3 Assessing the carbon dynamics and greenhouse gases production in natural and perturbed boreal aquatic systems: A bulk isotopie approach 43 3.1 Abstract 44 3.2 Introduction 45 3.3 Materials and methods 48 3.3.1 Study sites 48 3.3.2 Field sampling 52 3.3.3 Soil leaching experiment 54 3.3.4 DOC, total nitrogen and total phosphate measurements 54 3.3.5 Elemental and isotopie measurements 54 3.3.6 DOM-complexed iron 55 3.3.7 Statistical analyses 56 3.4 Results 56 3.4.1 Greenhouse gases 56 3.4.2 Water chemistry 59 3.4.3 Terrestrial and aquatic bulk organic matter analyses 63 3.4.4 Dissolved inorganic carbon (DIC) 68 3.4.5 POC isotopie variations 70 3.5 Discussion 73 3.5. 1 Using water chemistry and bulk analyses to study carbon cycling 73 3.5.2 Linking heterotrophy and primary productivity to DIC 76 3.5.3 In-lake bioprocesses affected by DOM cycling 77 3.6 Summary and implications 80 3.6.1 Effects ofmature reservoir operation on C cycling 80 3.6.2 Effects of wood harvesting on the aquatic cycle of carbon 81 3.6.3 General Implications 82 4 Assessing carbon and nitrogen dynamics in natural and perturbed boreal aquatic systems: An amino acid approach 85 Vili 4.1 Abstract 86 4.2 Introduction..... 88 4.3 Materials and Methods 92 4.3.1 Study sites 92 4.3.2 Field sampling 94 4.3.3 Elemental and isotopie measurements 96 4.3.4 Iron associated to DOM 96 4.3.5 Sedimentation rates 97 4.3.6 Amino acids measurements 97 4.3.7 Statistical Analysis 99 4.4 Results 100 4.4.1 Greenhouse gases and bulk organic matter analyses 100 4.4.2 L- and D-Amino acid analyses 105 4.5 Discussion 114 4.5.1 Sources of lacustrine OM 1 14 4.5.2 Changes in OM diagenetic state 1 17 4.5.3 Changes in bacterial abundance 119 4.5.4 Principal component analysis 123 5 The modulation ofthe carbon
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