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������������������������������������������������������������������ ���������������������������������������������� ������������������������������������������������� ������������������������������������������ ���������� ���������� ����� ���� ���� ������� ������� ����� ���� ����� ���������� ������������ ���������� ��� ���� � �� ������ � ����� �� � � ���� � ������ � � ���� �� �������������� � �� � � ���� � � � ������ � �� �� ������������� ����������������������������������������� ������������������������������� ���������������������� Cover: Illustrations of largemouth bass, and yellow perch have been supplied courtesy of the Ohio State Environmental Protection Agency. Sources of Mercury in Sediments, Water, and Fish of the Lakes of Whatcom County, Washington By Anthony J. Paulson Prepared in cooperation with the Whatcom County Health Department and the Washington State Department of Ecology Scientific Investigations Report 2004-5084 U.S. Department of the Interior U.S. Geological Survey U.S. Department of the Interior Gale A. Norton, Secretary U.S. Geological Survey Charles G. Groat, Director U.S. Geological Survey, Reston, Virginia: 2004 For sale by U.S. Geological Survey, Information Services Box 25286, Denver Federal Center Denver, CO 80225-0286 For more information about the USGS and its products: Telephone: 1-888-ASK-USGS World Wide Web: http://www.usgs.gov/ Any use of trade, product, or firm names in this publication is for descriptive purposes only and does not imply endorsement by the U.S. Government. Although this report is in the public domain, permission must be secured from the individual copyright owners to reproduce any copyrighted materials contained within this report. Suggested citation: Paulson, A.J., 2004, Sources of mercury in sediments, water, and fish of the Lakes of Whatcom County, Washington: U.S. Geological Survey Scientific Investigations Report 2004-5084, 98 p. iii Contents Abstract ……………………………………………………………………………………… 1 Introduction …………………………………………………………………………………… 1 Purpose and Scope ……………………………………………………………………… 2 Acknowledgments ……………………………………………………………………… 3 Description of Study Area …………………………………………………………………… 3 Study Methods ……………………………………………………………………………… 6 Evaluation of Possible Sources of Mercury to Lake Whatcom and Other Lakes in Whatcom County ……………………………………………………………………… 6 Atmospheric Inputs ……………………………………………………………………… 6 Deposition of Mercury from Non-Local Atmospheric Sources …………………… 6 Local Atmospheric Sources and Total Mercury Emission Rates …………………… 8 Municipal and Sludge Incinerators …………………………………………… 8 Chlor-Alkali Plant ……………………………………………………………… 10 Other Mercury Air Sources in Whatcom County ……………………………… 12 Model of Mercury Deposition to Lakes in Whatcom County from a Unit Mercury Emission ………………………………………………………… 12 Estimates of Mercury Deposition to Lakes in Whatcom County from Known Sources ……………………………………………………………… 15 Thermal Reduction Company, Inc. Municipal Waste Incinerator …………… 17 Olivine Corporation Municipal Waste Incinerator …………………………… 17 City of Bellingham Sewage Sludge Incinerator ……………………………… 21 Georgia-Pacific Chlor-Alkali Plant …………………………………………… 21 Summary of Deposition from Local Air Emissions …………………………… 22 Tributary Riverine Inputs ………………………………………………………………… 23 Ground-Water Sources ………………………………………………………………… 30 Mercury in Lake Whatcom and Other Lakes in Whatcom County …………………………… 31 Sediments ……………………………………………………………………………… 31 Surface Sediments ………………………………………………………………… 31 Mercury Sedimentation in Lakes …………………………………………………… 33 Water Column …………………………………………………………………………… 40 Fish ……………………………………………………………………………………… 40 Smallmouth Bass …………………………………………………………………… 43 Largemouth Bass …………………………………………………………………… 44 Cutthroat Trout ……………………………………………………………………… 46 Yellow Perch ……………………………………………………………………… 48 Brown Bullhead …………………………………………………………………… 49 Other Species ……………………………………………………………………… 49 Biogeochemical Behavior of Mercury in Lake Whatcom …………………………………… 51 Mass Balances of Mercury in Lake Whatcom ……………………………………………… 52 Suggestions for Future Studies ……………………………………………………………… 53 Summary and Conclusions …………………………………………………………………… 54 References Cited ……………………………………………………………………………… 55 iv Appendix A. Analysis of Mercury in Fish and Assessment of Quality of Data Used in the Report ……………………………………………………… 59 Appendix B. Estimates of Atmospheric Deposition to Lakes in Whatcom County for Sources Emitting a Hypothetical Unit of Mercury Emission in Bellingham, Ferndale, and at the Bellingham Airport ………………………… 63 Appendix C. Method for Calculating Missing Flow Data for the Tributaries of Lake Whatcom ………………………………………………………………… 72 Appendix D. Analysis of Core Sections and Estimates of Sedimentation Rates in Lakes in Whatcom County …………………………………………………… 73 v Figures 1. Map showing location of study area and lakes in Whatcom County, Washington ……………………………………………………… 2 2. Map showing location of the basins of Lake Whatcom and its tributaries, Whatcom County, Washington ………………………………… 5 3. Profile showing historical concentrations of mercury in ice core from Upper Fremont Glacier, Wyoming …………………………………… 7 4. Diagram showing timelines of local atmospheric sources of mercury …………… 8 5. Diagram showing concepts of a simple model of the deposition of mercury ……………………………………………………………… 14 6. Map showing location of sources of mercury emissions, sediment core sampling sites, and solid waste sites, with the 1996 wind field at Georgia-Pacific meteorological station superimposed, Bellingham, Washington …………………………………………… 15 7. Graphs showing estimates of atmospheric deposition of mercury as a function of times of significantly different operations for the three basins of Lake Whatcom and Lake Terrell and Fazon and Wiser Lakes, Whatcom County, Washington ………………………………… 19 8. Hydrographs showing daily mean flows of tributaries to Lake Whatcom, Washington, June 2002 – May 2003 ……………………………… 26 9. Graph showing correlation of total mercury and specific conductance in Olsen Creek, tributary to Lake Whatcom, Washington …………… 28 10. Graph showing relation of total organic carbon and total mercury to percentage of fines (<0.004 mm) in samples of surface sediments collected in 2002 near tributaries and in the three basins of Lake Whatcom, Washington …………………………………………………… 32 11. Graph showing relation of methyl-mercury to total organic carbon in samples of surface sediments from the three basins of Lake Whatcom, Washington, 2002 ……………………………………………… 33 12. Profiles showing relation of enrichment ratio of mercury with time in sediment cores from the three basins of Lake Whatcom, and Lake Terrell and Fazon and Wiser Lakes, Whatcom County, Washington, 2002 …………………………………………………………………… 37 13. Bar graph showing historical, pre-1964, peak and recent rates of mercury accumulation in core sections from Lake Whatcom, Washington ………………………………………………………………………… 39 14. Graphs showing estimated partitioning of mercury between the dissolved and particulate phases in five samples in the upper water column and two samples in the near-bottom water column of the three basins of Lake Whatcom, Washington ………………………………… 42 15. Graph showing relation of concentration of mercury in fillets to total length of smallmouth bass in Lake Whatcom, Washington ………………… 44 16. Graph showing relation of concentrations of mercury in fillets to total length of largemouth bass in selected lakes of Whatcom County, Washington. …………………………………………………… 45 vi Figures — Continued 17. Graph showing relation of concentration of mercury in fillets to total length of cutthroat trout in Lake Samish and the three basins of Lake Whatcom, Washington ……………………………………… 47 18. Graph showing relation of concentration of mercury in fillets to a conditioning factor for large cutthroat trout in Lake Whatcom, Washington ……………………………………………………… 47 19. Graph showing relation of concentration of mercury in fillets to total length of yellow perch in Tennant Lake and Lake Whatcom, Washington ……………………………………………………… 49 20. Graph showing relation of concentration of mercury to total length of brown bullhead in Lake Whatcom, Washington ………………………… 50 vii Tables 1. Statistics on lakes in Whatcom County, Washington ……………………………… 4 2. Measured deposition of atmospheric mercury (Hg) in the Pacific Northwest, 1997-2002 ……………………………………………………… 6 3. Rate of emission of mercury (Hg) and other characteristics related to local sources of mercury in Whatcom County, Washington …………… 9 4. Matrix of confidence category for estimates of mercury (Hg) deposition based on source of emission and speciation data ……………………… 16 5. Estimates of deposition rates of mercury to lakes in Whatcom County from local emission sources, Washington ……………………… 18 6. Summary of analyses of water samples from the mouth of the tributaries to Lake Whatcom, Washington, July 2002 to May 2003 ………………… 24 7. Concentrations of mercury (Hg) at the terminus of the Nooksack River diversion, Whatcom County, Washington, October 2001–August 2003 …………… 28 8. Annual loadings of mercury (Hg) to Lake Whatcom, Washington, from tributary inflows, June 2002 – May 2003 ……………………………………… 29 9. Summary of concentrations and sedimentation rates of mass, total organic carbon, mercury (Hg), lead, lead-210, cesium-137, and total organic carbon in sediment cores from lakes in Whatcom County, Washington ……………………………………………………… 34 10. Summary of analyses of mercury (Hg) in sediment cores from lakes in Whatcom County, Washington, September 2002 ………………………………… 36 11. Concentrations of total and dissolved mercury (Hg) and methyl-mercury in Lake Whatcom, Washington, October 2001 …………………… 41