Mercury source changes and food web shifts alter contamination signatures of predatory fish from Lake Michigan

Ryan F. Lepak; Joel C. Hoffman; Sarah E. Janssen; David P. Krabbenhoft; Jacob M. Ogorek; John F. DeWild; Michael T. Tate; Christopher L. Babiarz; Runsheng Yin; Elizabeth W. Murphy; Daniel R. Engstrom; James P. Hurley

doi:10.1073/pnas.1907484116

Mercury source changes and food web shifts alter contamination signatures of predatory fish from Lake Michigan

Ryan F. Lepak, Joel C. Hoffman, Sarah E. Janssen, David P. Krabbenhoft, Jacob M. Ogorek, John F. DeWild, Michael T. Tate, Christopher L. Babiarz, Runsheng Yin, Elizabeth W. Murphy, Daniel R. Engstrom, James P. Hurley

Research output: Contribution to journal › Article › peer-review

36 Scopus citations

Abstract

To understand the impact reduced mercury (Hg) loading and invasive species have had on methylmercury bioaccumulation in predator fish of Lake Michigan, we reconstructed bioaccumulation trends from a fish archive (1978 to 2012). By measuring fish Hg stable isotope ratios, we related temporal changes in Hg concentrations to varying Hg sources. Additionally, dietary tracers were necessary to identify food web influences. Through combined Hg, C, and N stable isotopic analyses, we were able to differentiate between a shift in Hg sources to fish and periods when energetic transitions (from dreissenid mussels) led to the assimilation of contrasting Hg pools (2000 to present). In the late 1980s, lake trout δ²⁰²Hg increased (0.4) from regulatory reductions in regional Hg emissions. After 2000, C and N isotopes ratios revealed altered food web pathways, resulting in a benthic energetic shift and changes to Hg bioaccumulation. Continued increases in δ²⁰²Hg indicate fish are responding to several United States mercury emission mitigation strategies that were initiated circa 1990 and continued through the 2011 promulgation of the Mercury and Air Toxics Standards rule. Unlike archives of sediments, this fish archive tracks Hg sources susceptible to bioaccumulation in Great Lakes fisheries. Analysis reveals that trends in fish Hg concentrations can be substantially affected by shifts in trophic structure and dietary preferences initiated by invasive species in the Great Lakes. This does not diminish the benefits of declining emissions over this period, as fish Hg concentrations would have been higher without these actions.

Original language	English (US)
Pages (from-to)	23600-23608
Number of pages	9
Journal	Proceedings of the National Academy of Sciences of the United States of America
Volume	116
Issue number	47
DOIs	https://doi.org/10.1073/pnas.1907484116
State	Published - Jan 1 2019

Bibliographical note

Funding Information:
aEnvironmental Chemistry and Technology Program, University of Wisconsin–Madison, Madison, WI 53706; bUS Geological Survey, Upper Midwest Water Science Center, USGS Mercury Research Laboratory, Middleton, WI 53562; cUS Environmental Protection Agency (US EPA) Office of Research and Development, Center for Computational Toxicology and Exposure, Great Lakes Toxicology and Ecology Division, Duluth, MN 55804; dState Key Laboratory of Ore Deposit Geochemistry, Institute of Geochemistry, Chinese Academy of Sciences, Guanshanhu District, 550081 Guiyang, Guizhou, China; eGreat Lakes National Program Office, US EPA, Chicago, IL 60604; fSt. Croix Watershed Research Station, Science Museum of Minnesota, Marine on St. Croix, MN 55047; gDepartment of Civil and Environmental Engineering, University of Wisconsin–Madison, Madison, WI 53706; and hUniversity of Wisconsin Aquatic Sciences Center, Madison, WI 53706

Funding Information:
the National Park Service and US EPA (Great Lakes Restoration Initiative Project #91). Ship support was provided by the University of Michigan/ National Oceanic and Atmospheric Administration R/V Laurentian and the US EPA R/V Lake Guardian. The views expressed in this paper are solely

Funding Information:
ACKNOWLEDGMENTS. This work was supported by the US EPA Great Lakes Restoration Initiative (Project GL-00E01139), the US Geological Survey (USGS) Toxic Substances Hydrology Program, and the US EPA Great Lakes Fish Monitoring and Surveillance Program (Elizabeth Murphy, Program Manager). Partial graduate student support was provided by the Wisconsin Alumni Research Foundation through the University of Wisconsin–Madison Graduate School (Award MSN165161) and the University of Wisconsin Water Resources Institute through a USGS-National Institutes for Water Resources fellowship (Award MSN197848). Lake Michigan sediment core collection was coordinated by Mark Edlund (St. Croix Watershed Research Station) and was supported by the Great Lakes Fishery Trust (Project 2008.960) and

Funding Information:
This work was supported by the US EPA Great Lakes Restoration Initiative (Project GL-00E01139), the US Geological Survey (USGS) Toxic Substances Hydrology Program, and the US EPA Great Lakes Fish Monitoring and Surveillance Program (Elizabeth Murphy, Program Manager). Partial graduate student support was provided by the Wisconsin Alumni Research Foundation through the University of Wisconsin?Madison Graduate School (Award MSN165161) and the University of Wisconsin Water Resources Institute through a USGS-National Institutes for Water Resources fellowship (Award MSN197848). Lake Michigan sediment core collection was coordinated by Mark Edlund (St. Croix Watershed Research Station) and was supported by the Great Lakes Fishery Trust (Project 2008.960) and the National Park Service and US EPA (Great Lakes Restoration Initiative Project #91). Ship support was provided by the University of Michigan/ National Oceanic and Atmospheric Administration R/V Laurentian and the US EPA R/V Lake Guardian. The views expressed in this paper are solely those of the authors and the content of the paper does not represent the views or position of the US EPA, but do represent the views of the USGS. Any use of trade, firm, or product, in this publication is for descriptive purposes only and does not imply endorsement by the US Government.

Publisher Copyright:
© 2019 National Academy of Sciences. All rights reserved.

Keywords

Fish
Invasive
Isotopes
Lake Michigan
Mercury

PubMed: MeSH publication types

Journal Article
Research Support, Non-U.S. Gov't
Research Support, U.S. Gov't, Non-P.H.S.

UN SDGs

This output contributes to the following UN Sustainable Development Goals (SDGs)

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10.1073/pnas.1907484116

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Lepak, R. F., Hoffman, J. C., Janssen, S. E., Krabbenhoft, D. P., Ogorek, J. M., DeWild, J. F., Tate, M. T., Babiarz, C. L., Yin, R., Murphy, E. W., Engstrom, D. R., & Hurley, J. P. (2019). Mercury source changes and food web shifts alter contamination signatures of predatory fish from Lake Michigan. Proceedings of the National Academy of Sciences of the United States of America, 116(47), 23600-23608. https://doi.org/10.1073/pnas.1907484116

Mercury source changes and food web shifts alter contamination signatures of predatory fish from Lake Michigan. / Lepak, Ryan F.; Hoffman, Joel C.; Janssen, Sarah E. et al.
In: Proceedings of the National Academy of Sciences of the United States of America, Vol. 116, No. 47, 01.01.2019, p. 23600-23608.

Research output: Contribution to journal › Article › peer-review

Lepak, RF, Hoffman, JC, Janssen, SE, Krabbenhoft, DP, Ogorek, JM, DeWild, JF, Tate, MT, Babiarz, CL, Yin, R, Murphy, EW, Engstrom, DR & Hurley, JP 2019, 'Mercury source changes and food web shifts alter contamination signatures of predatory fish from Lake Michigan', Proceedings of the National Academy of Sciences of the United States of America, vol. 116, no. 47, pp. 23600-23608. https://doi.org/10.1073/pnas.1907484116

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abstract = "To understand the impact reduced mercury (Hg) loading and invasive species have had on methylmercury bioaccumulation in predator fish of Lake Michigan, we reconstructed bioaccumulation trends from a fish archive (1978 to 2012). By measuring fish Hg stable isotope ratios, we related temporal changes in Hg concentrations to varying Hg sources. Additionally, dietary tracers were necessary to identify food web influences. Through combined Hg, C, and N stable isotopic analyses, we were able to differentiate between a shift in Hg sources to fish and periods when energetic transitions (from dreissenid mussels) led to the assimilation of contrasting Hg pools (2000 to present). In the late 1980s, lake trout δ202Hg increased (0.4) from regulatory reductions in regional Hg emissions. After 2000, C and N isotopes ratios revealed altered food web pathways, resulting in a benthic energetic shift and changes to Hg bioaccumulation. Continued increases in δ202Hg indicate fish are responding to several United States mercury emission mitigation strategies that were initiated circa 1990 and continued through the 2011 promulgation of the Mercury and Air Toxics Standards rule. Unlike archives of sediments, this fish archive tracks Hg sources susceptible to bioaccumulation in Great Lakes fisheries. Analysis reveals that trends in fish Hg concentrations can be substantially affected by shifts in trophic structure and dietary preferences initiated by invasive species in the Great Lakes. This does not diminish the benefits of declining emissions over this period, as fish Hg concentrations would have been higher without these actions.",

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note = "Funding Information: aEnvironmental Chemistry and Technology Program, University of Wisconsin–Madison, Madison, WI 53706; bUS Geological Survey, Upper Midwest Water Science Center, USGS Mercury Research Laboratory, Middleton, WI 53562; cUS Environmental Protection Agency (US EPA) Office of Research and Development, Center for Computational Toxicology and Exposure, Great Lakes Toxicology and Ecology Division, Duluth, MN 55804; dState Key Laboratory of Ore Deposit Geochemistry, Institute of Geochemistry, Chinese Academy of Sciences, Guanshanhu District, 550081 Guiyang, Guizhou, China; eGreat Lakes National Program Office, US EPA, Chicago, IL 60604; fSt. Croix Watershed Research Station, Science Museum of Minnesota, Marine on St. Croix, MN 55047; gDepartment of Civil and Environmental Engineering, University of Wisconsin–Madison, Madison, WI 53706; and hUniversity of Wisconsin Aquatic Sciences Center, Madison, WI 53706 Funding Information: the National Park Service and US EPA (Great Lakes Restoration Initiative Project #91). Ship support was provided by the University of Michigan/ National Oceanic and Atmospheric Administration R/V Laurentian and the US EPA R/V Lake Guardian. The views expressed in this paper are solely Funding Information: ACKNOWLEDGMENTS. This work was supported by the US EPA Great Lakes Restoration Initiative (Project GL-00E01139), the US Geological Survey (USGS) Toxic Substances Hydrology Program, and the US EPA Great Lakes Fish Monitoring and Surveillance Program (Elizabeth Murphy, Program Manager). Partial graduate student support was provided by the Wisconsin Alumni Research Foundation through the University of Wisconsin–Madison Graduate School (Award MSN165161) and the University of Wisconsin Water Resources Institute through a USGS-National Institutes for Water Resources fellowship (Award MSN197848). Lake Michigan sediment core collection was coordinated by Mark Edlund (St. Croix Watershed Research Station) and was supported by the Great Lakes Fishery Trust (Project 2008.960) and Funding Information: This work was supported by the US EPA Great Lakes Restoration Initiative (Project GL-00E01139), the US Geological Survey (USGS) Toxic Substances Hydrology Program, and the US EPA Great Lakes Fish Monitoring and Surveillance Program (Elizabeth Murphy, Program Manager). Partial graduate student support was provided by the Wisconsin Alumni Research Foundation through the University of Wisconsin?Madison Graduate School (Award MSN165161) and the University of Wisconsin Water Resources Institute through a USGS-National Institutes for Water Resources fellowship (Award MSN197848). Lake Michigan sediment core collection was coordinated by Mark Edlund (St. Croix Watershed Research Station) and was supported by the Great Lakes Fishery Trust (Project 2008.960) and the National Park Service and US EPA (Great Lakes Restoration Initiative Project #91). Ship support was provided by the University of Michigan/ National Oceanic and Atmospheric Administration R/V Laurentian and the US EPA R/V Lake Guardian. The views expressed in this paper are solely those of the authors and the content of the paper does not represent the views or position of the US EPA, but do represent the views of the USGS. Any use of trade, firm, or product, in this publication is for descriptive purposes only and does not imply endorsement by the US Government. Publisher Copyright: {\textcopyright} 2019 National Academy of Sciences. All rights reserved.",

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doi = "10.1073/pnas.1907484116",

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T1 - Mercury source changes and food web shifts alter contamination signatures of predatory fish from Lake Michigan

AU - Lepak, Ryan F.

AU - Hoffman, Joel C.

AU - Janssen, Sarah E.

AU - Krabbenhoft, David P.

AU - Ogorek, Jacob M.

AU - DeWild, John F.

AU - Tate, Michael T.

AU - Babiarz, Christopher L.

AU - Yin, Runsheng

AU - Murphy, Elizabeth W.

AU - Engstrom, Daniel R.

AU - Hurley, James P.

N1 - Funding Information: aEnvironmental Chemistry and Technology Program, University of Wisconsin–Madison, Madison, WI 53706; bUS Geological Survey, Upper Midwest Water Science Center, USGS Mercury Research Laboratory, Middleton, WI 53562; cUS Environmental Protection Agency (US EPA) Office of Research and Development, Center for Computational Toxicology and Exposure, Great Lakes Toxicology and Ecology Division, Duluth, MN 55804; dState Key Laboratory of Ore Deposit Geochemistry, Institute of Geochemistry, Chinese Academy of Sciences, Guanshanhu District, 550081 Guiyang, Guizhou, China; eGreat Lakes National Program Office, US EPA, Chicago, IL 60604; fSt. Croix Watershed Research Station, Science Museum of Minnesota, Marine on St. Croix, MN 55047; gDepartment of Civil and Environmental Engineering, University of Wisconsin–Madison, Madison, WI 53706; and hUniversity of Wisconsin Aquatic Sciences Center, Madison, WI 53706 Funding Information: the National Park Service and US EPA (Great Lakes Restoration Initiative Project #91). Ship support was provided by the University of Michigan/ National Oceanic and Atmospheric Administration R/V Laurentian and the US EPA R/V Lake Guardian. The views expressed in this paper are solely Funding Information: ACKNOWLEDGMENTS. This work was supported by the US EPA Great Lakes Restoration Initiative (Project GL-00E01139), the US Geological Survey (USGS) Toxic Substances Hydrology Program, and the US EPA Great Lakes Fish Monitoring and Surveillance Program (Elizabeth Murphy, Program Manager). Partial graduate student support was provided by the Wisconsin Alumni Research Foundation through the University of Wisconsin–Madison Graduate School (Award MSN165161) and the University of Wisconsin Water Resources Institute through a USGS-National Institutes for Water Resources fellowship (Award MSN197848). Lake Michigan sediment core collection was coordinated by Mark Edlund (St. Croix Watershed Research Station) and was supported by the Great Lakes Fishery Trust (Project 2008.960) and Funding Information: This work was supported by the US EPA Great Lakes Restoration Initiative (Project GL-00E01139), the US Geological Survey (USGS) Toxic Substances Hydrology Program, and the US EPA Great Lakes Fish Monitoring and Surveillance Program (Elizabeth Murphy, Program Manager). Partial graduate student support was provided by the Wisconsin Alumni Research Foundation through the University of Wisconsin?Madison Graduate School (Award MSN165161) and the University of Wisconsin Water Resources Institute through a USGS-National Institutes for Water Resources fellowship (Award MSN197848). Lake Michigan sediment core collection was coordinated by Mark Edlund (St. Croix Watershed Research Station) and was supported by the Great Lakes Fishery Trust (Project 2008.960) and the National Park Service and US EPA (Great Lakes Restoration Initiative Project #91). Ship support was provided by the University of Michigan/ National Oceanic and Atmospheric Administration R/V Laurentian and the US EPA R/V Lake Guardian. The views expressed in this paper are solely those of the authors and the content of the paper does not represent the views or position of the US EPA, but do represent the views of the USGS. Any use of trade, firm, or product, in this publication is for descriptive purposes only and does not imply endorsement by the US Government. Publisher Copyright: © 2019 National Academy of Sciences. All rights reserved.

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N2 - To understand the impact reduced mercury (Hg) loading and invasive species have had on methylmercury bioaccumulation in predator fish of Lake Michigan, we reconstructed bioaccumulation trends from a fish archive (1978 to 2012). By measuring fish Hg stable isotope ratios, we related temporal changes in Hg concentrations to varying Hg sources. Additionally, dietary tracers were necessary to identify food web influences. Through combined Hg, C, and N stable isotopic analyses, we were able to differentiate between a shift in Hg sources to fish and periods when energetic transitions (from dreissenid mussels) led to the assimilation of contrasting Hg pools (2000 to present). In the late 1980s, lake trout δ202Hg increased (0.4) from regulatory reductions in regional Hg emissions. After 2000, C and N isotopes ratios revealed altered food web pathways, resulting in a benthic energetic shift and changes to Hg bioaccumulation. Continued increases in δ202Hg indicate fish are responding to several United States mercury emission mitigation strategies that were initiated circa 1990 and continued through the 2011 promulgation of the Mercury and Air Toxics Standards rule. Unlike archives of sediments, this fish archive tracks Hg sources susceptible to bioaccumulation in Great Lakes fisheries. Analysis reveals that trends in fish Hg concentrations can be substantially affected by shifts in trophic structure and dietary preferences initiated by invasive species in the Great Lakes. This does not diminish the benefits of declining emissions over this period, as fish Hg concentrations would have been higher without these actions.

AB - To understand the impact reduced mercury (Hg) loading and invasive species have had on methylmercury bioaccumulation in predator fish of Lake Michigan, we reconstructed bioaccumulation trends from a fish archive (1978 to 2012). By measuring fish Hg stable isotope ratios, we related temporal changes in Hg concentrations to varying Hg sources. Additionally, dietary tracers were necessary to identify food web influences. Through combined Hg, C, and N stable isotopic analyses, we were able to differentiate between a shift in Hg sources to fish and periods when energetic transitions (from dreissenid mussels) led to the assimilation of contrasting Hg pools (2000 to present). In the late 1980s, lake trout δ202Hg increased (0.4) from regulatory reductions in regional Hg emissions. After 2000, C and N isotopes ratios revealed altered food web pathways, resulting in a benthic energetic shift and changes to Hg bioaccumulation. Continued increases in δ202Hg indicate fish are responding to several United States mercury emission mitigation strategies that were initiated circa 1990 and continued through the 2011 promulgation of the Mercury and Air Toxics Standards rule. Unlike archives of sediments, this fish archive tracks Hg sources susceptible to bioaccumulation in Great Lakes fisheries. Analysis reveals that trends in fish Hg concentrations can be substantially affected by shifts in trophic structure and dietary preferences initiated by invasive species in the Great Lakes. This does not diminish the benefits of declining emissions over this period, as fish Hg concentrations would have been higher without these actions.

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KW - Invasive

KW - Isotopes

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KW - Mercury

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Mercury source changes and food web shifts alter contamination signatures of predatory fish from Lake Michigan

Abstract

Bibliographical note

Keywords

PubMed: MeSH publication types

UN SDGs

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