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EFFECTS OF CLIMATE CHANGE ON MERCURY CONCENTRATIONS IN ARCTIC CHAR (SALVELINUSALPINUS) IN THE HIGH ARCTIC A Thesis Presented to The Faculty of Graduate Studies of The University of Guelph by NIKOLAUS GANTNER In partial fulfilment of requirements for the degree of Doctor of Philosophy November, 2008 © Nikolaus Gantner, 2008 Library and Bibliotheque et 1*1 Archives Canada Archives Canada Published Heritage Direction du Branch Patrimoine de I'edition 395 Wellington Street 395, rue Wellington Ottawa ON K1A0N4 Ottawa ON K1A0N4 Canada Canada Your file Votre reference ISBN: 978-0-494-47590-4 Our file Notre reference ISBN: 978-0-494-47590-4 NOTICE: AVIS: The author has granted a non L'auteur a accorde une licence non exclusive exclusive license allowing Library permettant a la Bibliotheque et Archives and Archives Canada to reproduce, Canada de reproduire, publier, archiver, publish, archive, preserve, conserve, sauvegarder, conserver, transmettre au public communicate to the public by par telecommunication ou par Plntemet, prefer, telecommunication or on the Internet, distribuer et vendre des theses partout dans loan, distribute and sell theses le monde, a des fins commerciales ou autres, worldwide, for commercial or non sur support microforme, papier, electronique commercial purposes, in microform, et/ou autres formats. paper, electronic and/or any other formats. The author retains copyright L'auteur conserve la propriete du droit d'auteur ownership and moral rights in et des droits moraux qui protege cette these. this thesis. Neither the thesis Ni la these ni des extraits substantiels de nor substantial extracts from it celle-ci ne doivent etre imprimes ou autrement may be printed or otherwise reproduits sans son autorisation. reproduced without the author's permission. In compliance with the Canadian Conformement a la loi canadienne Privacy Act some supporting sur la protection de la vie privee, forms may have been removed quelques formulaires secondaires from this thesis. ont ete enleves de cette these. While these forms may be included Bien que ces formulaires in the document page count, aient inclus dans la pagination, their removal does not represent il n'y aura aucun contenu manquant. any loss of content from the thesis. Canada ABSTRACT EFFECTS OF CLIMATE CHANGE ON MERCURY CONCENTRATIONS IN ARCTIC CHAR (SAL VELINUS ALPINUS) IN THE HIGH ARCTIC Nikolaus Gantner, MSc Advisors: University of Guelph, 2008 Professor Keith Solomon, PhD Professor Derek Muir, PhD Professor Michael Power, PhD Professor Dr. Roland Psenner This thesis is an investigation of linkages of climate change and mercury concentrations in landlocked Arctic char and underlying food webs in Canadian Arctic lakes. Although the neurotoxin mercury is globally present in all environments, temporal and spatial trends in aquatic biota are often inconsistent, or do not exist for remote environments. Knowledge gaps include the influence of abiotic factors, possibly climate, and food web parameters on mercury accumulation in top predators. Furthermore, anthropogenic and natural mercury present in the environment are not well differentiated. To address these research needs, we collected landlocked Arctic char from 27 systems and food web organism from 18 lakes, and recorded abiotic lake characteristics expected to influence mercury cycling. Total mercury (THg) and monomethylmercury (MeHg) concentrations, and stable isotopes of carbon (S13C), nitrogen (§15N), and mercury (5xHg) were determined. Relationships among these measures and with environmental characteristics were investigated. A temporal trend of mercury in Arctic char (muscle tissue) from the largest lake in the Canadian High Arctic from an existing dataset and newly collected char was investigated. Two abundant char morphotypes from Lake Hazen differed in mercury concentrations, and the resulting variability was accounted for using a statistical adjustment. Mercury concentrations did not change over the 16-year period (1990-2006), which is consistent with nearby measurements of gaseous elemental mercury at Alert (Nunavut, Canada). Food chain lengths (FCL) of 18 lakes were characterized, biomagnification of mercury was investigated using SI5N, and results compared among regions. Food web biomagnification was confirmed using trophic magnification factors (TMFs) in 18 Arctic char bearing lakes (TMFs 3.5 - 64.3). Benthic coupling was apparent from char 813C signatures that resembled 613C in chironomid midges. TMFs and FCL partly explained THg in adult char, but no latitudinal or other climatic trend was apparent. Mercury concentrations in adult Arctic char were positively related to catchment-to-lake area, and intra-regional, and regional differences in Hg in Arctic char were determined. No climatic factor we investigated was found to affect Hg in char directly; however, predicted climatic changes could affect THg in char indirectly through changes in the catchment (such as melting of permafrost). Stable isotope ratios of mercury revealed region specific mass-independent fractionation (MIF) of up to ~ 4.5 %o in Arctic char, which did reflect sediment ratios with a constant offset (MIF-factor). High MIF in zooplankton possibly reflected mercury assimilated from the water column. Char from Lake Pingualuk, known pelagic feeders, had high MIF, possibly reflecting an atmospheric Hg signal. PREFACE This thesis has been organized as a series of manuscripts. Chapter 2 has been accepted for publication in Environmental Toxicology and Chemistry and is currently in press. Chapters 3, 4, and 5 are in intended for submission to Environmental Toxicology and Chemistry (Chapter 3, 4), and Environmental Science and Technology (Chapter 5). A general introduction (Chapter 1) and overall conclusion (Chapter 6) bracket the research chapters. As a result, some repetition of introductory and methodological material could not be avoided. Specific contributions of individual co-authors are highlighted where necessary; otherwise, co-authorship does represent intellectual contribution to the publication. All manuscripts listed below were written by Nikolaus Gantner, as indicated by primary authorship. Editorial comments and points of discussion were contributed by Drs Keith R. Solomon, Derek Muir, Michael Power, and Roland Psenner. Chapter 2: Gantner N, Power, M, Babaluk, J, Reist, JD, Kock, G, Lockhart, WL, Solomon, KR, and Muir, DCG 2009a. Temporal trends of mercury, cesium, potassium, selenium, and thallium in Arctic Char (Salvelinus alpinus) from Lake Hazen (Nunavut): Effects of trophic position, size and age. Environmental Toxicology and Chemistry (in press, accepted Aug 14 08). > J Babaluk and JD Reist (both Freshwater institute, Winnipeg, MB, Canada) determined the ages of Arctic char, and provided comments on the manuscript > G Kock (Austrian Academy of Science) assisted in the collection of Arctic char. > Mercury data and fish biodata from 1990 and 1992 were provided by WL Lockhart (North-South Consulting, Winnipeg, MB, Canada) i Chapter 3: Gantner, N, Power, M, Lawson, G, Iqaluk, D, Meili, M, Kock, G, Borg, H, Sundbom, M, Solomon, KR, and Muir, DCG; 2009b; Mercury Concentrations in Landlocked Arctic char (Salvelinus alpinus) from the Canadian High Arctic: Part I - insights from trophic relationships in 18 lakes; in prep for submission to Environmental Toxicology and Chemistry. > G Lawson (NWRI, Burlington, ON) conducted the MeHg analysis in biota > D Iqaluk assisted in char and food web collection at 15 sites between 2005-2007 > M Meili (Stockholm University, Sweden) provided TNW99 Arctic char THg and stable isotope data, and zooplankton samples for THg and MeHg analysis > G K6ck aided in field collections 2005 and 2007 > H Borg, M Sundbom (both Stockholm University, Sweden) made TNW99 Arctic char data (HB) and zooplankton samples (MS) available Chapter 4: Gantner, N, Muir, DCG, Power, M, Reist JD, Babaluk, J, Iqaluk, D, Michaud, W, Meili, M, Kock, G, Dempson JB, Borg H, Hammar J, and Solomon, KR; 2009c. Mercury Concentrations in Landlocked Arctic char {Salvelinus alpinus) in the Canadian High Arctic: Part II - Spatial comparison of 27 populations; in prep for submission to Environmental Toxicology and Chemistry > JD Reist (Freshwater Institute, Winnipeg) aided char sampling of 2007, TNW99 > J Babaluk (Freshwater Institute, Winnipeg) coordinated age-determination of char, and provided logistical support > D Iqaluk assisted in char and food web collection at 15 sites between 2005-2007 ii > W Michaud assisted in fish dissections (2007) and stable isotope analysis > M Meili, H Borg, M Sundbom (see Chapter 3) > G Kock provided gill nets and aided in char collections and dissections 2001, 2005-2007 > JB Dempson supplied 2007 char samples from Labrador (3 lakes) > J Hammar (Institute of Freshwater Research, Drottningholm, Sweden) made TNW99 Arctic char data available Chapter 5: Gantner, N, Hintelmann, H, Zheng, W, and Muir, DCG; 2009d; Fractionation and variations of mercury isotopes in Arctic lake food webs; in prep for submission to Environmental Science and Technology. > All MC-ICP-MS work was conducted in the laboratory of H Hintelmann (Trent University, ON, Canada), who also provided comments on the manuscript > W Zheng (Trent University, ON, Canada) aided with analytical method, and commented on the manuscript in ACKNOWLEDGMENTS The privilege to set foot into the Canadian Arctic is tremendous; greater still is being able to follow one's passions in this remote and pristine region. Dr. Derek Muir, thank you for this fantastic