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Mercury Dynamics in Sulfide-Rich Sediments: Geochemical Influence on Contaminant Mobilization and Methylation Within the Penobscot River Estuary, Maine, USA Karen A

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Mercury Dynamics in Sulfide-Rich Sediments: Geochemical Influence on Contaminant Mobilization and Methylation Within the Penobscot River Estuary, Maine, USA Karen A The University of Maine DigitalCommons@UMaine Electronic Theses and Dissertations Fogler Library 2007 Mercury Dynamics in Sulfide-Rich Sediments: Geochemical Influence on Contaminant Mobilization and Methylation within the Penobscot River Estuary, Maine, USA Karen A. Merritt University of Maine - Main Follow this and additional works at: http://digitalcommons.library.umaine.edu/etd Part of the Civil and Environmental Engineering Commons Recommended Citation Merritt, Karen A., "Mercury Dynamics in Sulfide-Rich Sediments: Geochemical Influence on Contaminant Mobilization and Methylation within the Penobscot River Estuary, Maine, USA" (2007). Electronic Theses and Dissertations. 99. http://digitalcommons.library.umaine.edu/etd/99 This Open-Access Dissertation is brought to you for free and open access by DigitalCommons@UMaine. It has been accepted for inclusion in Electronic Theses and Dissertations by an authorized administrator of DigitalCommons@UMaine. MERCURY DYNAMICS IN SULFIDE-RICH SEDIMENTS: GEOCHEMICAL INFLUENCE ON CONTAMINANT MOBILIZATION AND METHYLATION WITHIN THE PENOBSCOT RIVER ESTUARY, MAINE, USA By Karen A. Merritt B.A. Carleton College, 1989 M.S. University of Maine, 2002 M.S. University of Maine, 2006 A THESIS Submitted in Partial Fulfillment of the Requirements for the Degree of Doctor of Philosophy (in Civil Engineering) August, 2007 Advisory Committee: Aria Amirbahman, Associate Professor of Civil Engineering, Advisor Jean MacRae, Associate Professor of Civil Engineering Lawrence Mayer, Professor of Oceanography Stephen Norton, Professor of Earth Sciences Daniel Belknap, Professor of Earth Sciences MERCURY DYNAMICS IN SULFIDE-RICH SEDIMENTS: GEOCHEMICAL INFLUENCE ON CONTAMINANT MOBILIZATION AND METHYLATION WITHIN THE PENOBSCOT RIVER ESTUARY, MAINE, USA By Karen A. Merritt Thesis Advisor: Dr. Aria Amirbahman An Abstract for the Thesis Presented In Partial Fulfillment of the Requirements for the Degree of Doctor of Philosophy (in Civil Engineering) August, 2007 Research concerning the fate and biogeochemical cycling of mercury (Hg) within coastal ecosystems has suggested that microbially-mediated diagenetic processes control Hg mobilization and that ligands with strong affinity for Hg control Hg partitioning between the dissolved and particulate phases. Of specific further concern is the likelihood that Hg sequestered in coastal marine sediments may be efficiently methylated to highly toxic methylmercury (MeHg), thereby placing exposed organisms at significant risk of MeHg bioaccumulation. We have studied total dissolved Hg (HgT) and methylmercury (MeHg) cycling in the sediments of the Penobscot River estuary in Maine, USA using a combination of equilibrium porewater samplers, kinetic modeling, and Hg-specific reactive gels. The Penobscot estuary has been subject to Hg contamination from multiple industries including a recently closed chlor-alkali production facility. Pore water depth profiles for the Penobscot estuary are divisible into kinetically discrete intervals with respect to both Hgr and MeHg dynamics. Modeling results suggest that (1) while estuary sediments act as a net sink for particulate Hg inputs they may simultaneously function as a source of dissolved Hg to the overlying water and (2) dominant MeHg production occurs at shallow sediment depths, with the sharp decrease in porewater Mel lg concentration observed near the sediment water interface (SWI) likely explained by active demethylation. Intact sediment cores were incubated in the laboratory under various hydrodynamic regimes to assess the extent to which MeHg profiles (such as those just described) are sensitive to variation in geochemical and/or hydrodynamic conditions. Results demonstrate that ponding regimes change the location of the redoxcline and affect the sediment depth at which maximum net methylation occurs. Moreover, induced shoaling of the redoxcline demonstrates the potential for heightened MeHg efflux from the sediment. This flux may represent a distinct aqueous phase exposure pathway for coastal biota. The lability of porewater and sediment Hg was further examined by deploying mercapto-substituted siloxane gels within estuary sediments. The resultant observations of low general Hg reactivity support the hypothesis that porewater Hg may be defined as a function of porewater ligand production, highlighting the importance of microbially-mediated diagenesis in controlling Hg cycling within estuary sediments. ACKNOWLEDGEMENTS I thank the U.S. EPA STAR Fellowship Program, the Robert and Patricia Switzer Foundation, Maine Sea Grant, and the NOAA Saltonstall-Kennedy Program for funding this research. For use of laboratory space and equipment plus endless help with protocol development and sample analyses I thank the Sawyer Environmental Chemistry Research Laboratory. Specifically—to John Cangelosi, Clive Devoy, Karen Small, and Tiffany Wilson, thank you all for letting me clatter around in your lab. I hope I kept the chaos to something of a minimum. Thanks also to the folks at the Advanced Manufacturing Center, specifically Tom Christensen and Brian Barker, for all your help making gizmos. Tom—I appreciate your willingness to listen to yet another crazy deployment idea with a straight face. You folks made much of the sampling equipment required for this project to succeed [to the extent that it has] and I know that we often made things more complicated than they needed to be. To my office mates—Jennifer Weldon, Bjorn Lake, Brett Holmes, and Melinda Diehl, plus Dianne Kopec—thank you all for your help with field work and for making the office the positive place that it's been over these last several years. To Aria—thanks for being the finest dissertation advisor on the planet. I've really enjoyed working with you and admire and respect you as both a scientist and a person. Thank you for taking on this project and thank you even more for continually demonstrating what quality looks like. To Merrill Garrett, Peter Huang, and John Swalec—you all know what you did. Thank you for getting me this far. ii Finally and most significantly of all—thank you, Elliot, for absolutely everything. When 1 woke up that day and announced that it was time to go back to graduate school you rearranged many things to make it possible. I want you to know that I saw all that you did and I appreciate it beyond measure. As Joe Strummer said: without your love I won't make it through. in TABLE OF CONTENTS ACKNOWLEDGEMENTS ii LIST OF TABLES viii LIST OF FIGURES ix PREFACE x GLOSSARY OF TERMS xiv CHAPTER 1. Mercury dynamics in sulfide-rich sediments: geochemical influence on mercury mobilization within the Penobscot River Estuary, Maine, USA 1 1.1. Abstract 2 1.2. Introduction 3 1.3. Materials and Methods 6 1.3.1. Sediment Solid Phase 6 1.3.2. Porewater 10 1.3.3. Modeling 13 1.4. Results and Discussion 19 1.4.1. Sediment Solid Phase 19 1.4.2. Porewater Thermodynamics 20 iv 1.4.3. Porewater Kinetics 25 1.4.3.1. Fe(II) 25 1.4.3.2. S(-II) 28 1.4.3.3. HgT 28 1.5. Implications 35 2. Methylmercury cycling in estuarine sediment porewaters (Penobscot River Estuary, Maine, USA) 37 2.1. Abstract 38 2.2. Introduction 39 2.3. Materials and Methods 41 2.3.1. Sediment Solid Phase 41 2.3.2. Porewater 42 2.3.3. Intact Sediment Column Experiment 44 2.3.4. Modeling 46 2.4. Results and Discussion 48 2.4.1. Field Data 48 2.4.1.1. Porewater 48 2.4.1.2. Sediment Solid Phase 51 2.4.2. Column Data 51 v 2.4.3. Porewater Kinetics 56 2.4.3.1. Field Data 56 2.4.3.2. Intact Sediment Column Experiment 63 2.5. Implications 66 3. Mercury mobilization in estuarine sediment porewaters: a diffusive gel time-series study 68 3.1. Abstract 69 3.2. Introduction 70 3.3. Materials and Methods 74 3.3.1. SiloxaneGels 74 3.3.2. Porewater 76 3.3.3. Gel Data Modeling 76 3.3.4. Exchangeable Hg 78 3.4. Results and Discussion 80 3.4.1. SiloxaneGels 80 3.4.1.1. Zone A Data 80 3.4.1.2. Zone B Data 83 3.4.2. DIFS Modeling 87 3.5. Implications 89 vi 4. Mercury methylation dynamics in estuarine and marine sediments: a critical review 90 4.1. Abstract 91 4.2. Introduction 91 4.3. Metabolism-Related Influence on Mercury Methylation Rate 100 4.4. Speciation-Related Influence on Mercury Methylation Rate 106 4.5. Demethylation Dynamics 114 4.6. Conclusions 119 5. Research Implications for the Penobscot River Estuary, Maine, USA 123 BIBLIOGRAPHY 127 APPENDIX 143 BIOGRAPHY OF THE AUTHOR 172 vi i LIST OF TABLES Table 1.1. Equilibrium constants for reactions considered in this study 14 Table 1.2. Constants and terms for PROFILE modeling 17 Table 2.1. Output terms for PROFILE modeling of field MeHg data 60 Table 3.1. Conditional distribution coefficients for mercury extractions 88 Table A.l. 2004 Field Data-Short Cores 144 Table A.2. 2005 Field Data from Dialysis Samplers 145 Table A.3. 2006 Field Data from Dialysis Samplers 147 Table A.4. Sediment Solid Phase Data 2005-2006 149 Table A.5. Gamma Count + Sediment MeHg Data 151 Table A.6. Siloxane Gel Uptake Data 153 Table A.7. DIFS Model Output 154 Table A.8. 2006 Column Experiment-Porewater and Sediment Data 156 Table A.9. PROFILE Output 158 Table A. 10. 2005 Column Experiment-Porewater Data 170 vm f. LIST OF FIGURES Figure 1.1. Field sampling locations within the Penobscot River Estuary, Maine, USA 7 Figure 1.2. Spatial and depth variation in sediment Hg concentration for sampling sites in the Penobscot River Estuary 21 Figure 1.3. Porewater profiles and diagenetic modeling 22 Figure 1.4. Depth-dependent DOC spectral properties plus alkalinity as a function of DOC concentration 24 Figure 1.5. Porewater profiles and diagenetic modeling for HgT 26 Figure 2.1. Field porewater profiles collected with close-interval dialysis samplers 49 Figure 2.2.
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