Skip to main content

Thank you for visiting nature.com. You are using a browser version with limited support for CSS. To obtain the best experience, we recommend you use a more up to date browser (or turn off compatibility mode in Internet Explorer). In the meantime, to ensure continued support, we are displaying the site without styles and JavaScript.

  • Article
  • Published:

A vegetation control on seasonal variations in global atmospheric mercury concentrations

Abstract

Anthropogenic mercury emissions are transported through the atmosphere as gaseous elemental mercury (Hg(0)) before they are deposited to Earth’s surface. Strong seasonality in atmospheric Hg(0) concentrations in the Northern Hemisphere has been explained by two factors: anthropogenic Hg(0) emissions are thought to peak in winter due to higher energy consumption, and atmospheric oxidation rates of Hg(0) are faster in summer. Oxidation-driven Hg(0) seasonality should be equally pronounced in the Southern Hemisphere, which is inconsistent with observations of constant year-round Hg(0) levels. Here, we assess the role of Hg(0) uptake by vegetation as an alternative mechanism for driving Hg(0) seasonality. We find that at terrestrial sites in the Northern Hemisphere, Hg(0) co-varies with CO2, which is known to exhibit a minimum in summer when CO2 is assimilated by vegetation. The amplitude of seasonal oscillations in the atmospheric Hg(0) concentration increases with latitude and is larger at inland terrestrial sites than coastal sites. Using satellite data, we find that the photosynthetic activity of vegetation correlates with Hg(0) levels at individual sites and across continents. We suggest that terrestrial vegetation acts as a global Hg(0) pump, which can contribute to seasonal variations of atmospheric Hg(0), and that decreasing Hg(0) levels in the Northern Hemisphere over the past 20 years can be partly attributed to increased terrestrial net primary production.

This is a preview of subscription content, access via your institution

Access options

Buy this article

Prices may be subject to local taxes which are calculated during checkout

Fig. 1: Time records of atmospheric Hg(0) and CO2 concentrations.
Fig. 2: Effect of latitude on Hg(0) seasonality.
Fig. 3: Effect of vegetation activity on atmospheric Hg(0) and CO2 concentration.
Fig. 4: Seasonal variation of Hg emissions, vegetation activity and atmospheric Hg(0) concentrations.

Similar content being viewed by others

References

  1. Krabbenhoft, D. P. & Sunderland, E. M. Global change and mercury. Science 341, 1457–1458 (2013).

    Article  Google Scholar 

  2. Driscoll, C. T., Mason, R. P., Chan, H. M., Jacob, D. J. & Pirrone, N. Mercury as a global pollutant: sources, pathways, and effects. Environ. Sci. Technol. 47, 4967–4983 (2013).

    Article  Google Scholar 

  3. Temme, C. et al. Trend, seasonal and multivariate analysis study of total gaseous mercury data from the Canadian Atmospheric Mercury Measurement Network (CAMNet). Atmos. Environ. 41, 5423–5441 (2007).

    Article  Google Scholar 

  4. Fu, X. W. et al. Observations of atmospheric mercury in China: a critical review. Atmos. Chem. Phys. 15, 9455–9476 (2015).

    Article  Google Scholar 

  5. Weigelt, A. et al. Analysis and interpretation of 18 years of mercury observations since 1996 at Mace Head, Ireland. Atmos. Environ. 100, 85–93 (2015).

    Article  Google Scholar 

  6. Sprovieri, F. et al. Atmospheric mercury concentrations observed at ground-based monitoring sites globally distributed in the framework of the GMOS network. Atmos. Chem. Phys. 16, 11915–11935 (2016).

    Article  Google Scholar 

  7. Holmes, C. D. et al. Global atmospheric model for mercury including oxidation by bromine atoms. Atmos. Chem. Phys. 10, 12037–12057 (2010).

    Article  Google Scholar 

  8. Song, S. et al. Top-down constraints on atmospheric mercury emissions and implications for global biogeochemical cycling. Atmos. Chem. Phys. 15, 7103–7125 (2015).

    Article  Google Scholar 

  9. Horowitz, H. M. et al. A new mechanism for atmospheric mercury redox chemistry: implications for the global mercury budget. Atmos. Chem. Phys. 17, 6353–6371 (2017).

    Article  Google Scholar 

  10. Selin, N. E. et al. Chemical cycling and deposition of atmospheric mercury: global constraints from observations. J. Geophys. Res. 112, D02308 (2007).

    Article  Google Scholar 

  11. Slemr, F. et al. Comparison of mercury concentrations measured at several sites in the Southern Hemisphere. Atmos. Chem. Phys. 15, 3125–3133 (2015).

    Article  Google Scholar 

  12. Khalil, M. A. K. & Rasmussen, R. A. Sources, sinks, and seasonal cycles of atmospheric methane. J. Geophys. Res. Oceans 88, 5131–5144 (1983).

    Article  Google Scholar 

  13. Rea, A. W., Lindberg, S. E., Scherbatskoy, T. & Keeler, G. J. Mercury accumulation in foliage over time in two northern mixed-hardwood forests. Water Air Soil Pollut. 133, 49–67 (2002).

    Article  Google Scholar 

  14. St Louis, V. L. et al. Importance of the forest canopy to fluxes of methyl mercury and total mercury to boreal ecosystems. Environ. Sci. Technol. 35, 3089–3098 (2001).

    Article  Google Scholar 

  15. Lindberg, S. et al. A synthesis of progress and uncertainties in attributing the sources of mercury in deposition. Ambio 36, 19–32 (2007).

    Article  Google Scholar 

  16. Smith-Downey, N. V., Sunderland, E. M. & Jacob, D. J. Anthropogenic impacts on global storage and emissions of mercury from terrestrial soils: insights from a new global model. J. Geophys. Res. Biogeosci. 115, G03008 (2010).

    Article  Google Scholar 

  17. Obrist, D. Atmospheric mercury pollution due to losses of terrestrial carbon pools? Biogeochemistry 85, 119–123 (2007).

    Article  Google Scholar 

  18. Amos, H. M., Jacob, D. J., Streets, D. G. & Sunderland, E. M. Legacy impacts of all-time anthropogenic emissions on the global mercury cycle. Glob. Biogeochem. Cycles 27, 410–421 (2013).

    Article  Google Scholar 

  19. Zhang, L. et al. The estimated six-year mercury dry deposition across North America. Environ. Sci. Technol. 50, 12864–12873 (2016).

    Article  Google Scholar 

  20. Agnan, Y., Le Dantec, T., Moore, C. W., Edwards, G. C. & Obrist, D. New constraints on terrestrial surface-atmosphere fluxes of gaseous elemental mercury using a global database. Environ. Sci. Technol. 50, 507–524 (2016).

    Article  Google Scholar 

  21. Laacouri, A., Nater, E. A. & Kolka, R. K. Distribution and uptake dynamics of mercury in leaves of common deciduous tree species in Minnesota, U.S.A. Environ. Sci. Technol. 47, 10462–10470 (2013).

    Article  Google Scholar 

  22. Obrist, D. et al. Tundra uptake of atmospheric elemental mercury drives Arctic mercury pollution. Nature 547, 201–204 (2017).

    Article  Google Scholar 

  23. Graydon, J. A., St Louis, V. L., Lindberg, S. E., Hintelmann, H. & Krabbenhoft, D. P. Investigation of mercury exchange between forest canopy vegetation and the atmosphere using a new dynamic chamber. Environ. Sci. Technol. 40, 4680–4688 (2006).

    Article  Google Scholar 

  24. Wang, X., Bao, Z., Lin, C. J., Yuan, W. & Feng, X. Assessment of global mercury deposition through litterfall. Environ. Sci. Technol. 50, 8548–8557 (2016).

    Article  Google Scholar 

  25. Zhang, Y. et al. Observed decrease in atmospheric mercury explained by global decline in anthropogenic emissions. Proc. Natl Acad. Sci. USA 113, 526–531 (2016).

    Article  Google Scholar 

  26. Demers, J. D., Blum, J. D. & Zak, D. R. Mercury isotopes in a forested ecosystem: implications for air-surface exchange dynamics and the global mercury cycle. Glob. Biogeochem. Cycles 27, 222–238 (2013).

    Article  Google Scholar 

  27. Enrico, M. et al. Atmospheric mercury transfer to peat bogs dominated by gaseous elemental mercury dry deposition. Environ. Sci. Technol. 50, 2405–2412 (2016).

    Article  Google Scholar 

  28. Jiskra, M. et al. Mercury deposition and re-emission pathways in boreal forest soils investigated with Hg isotope signatures. Environ. Sci. Technol. 49, 7188–7196 (2015).

    Article  Google Scholar 

  29. Keeling, C. D. et al. Atmospheric carbon dioxide variations at Manua Lao observatory, Hawaii. Tellus 28, 538–551 (1976).

    Google Scholar 

  30. Keeling, C. D., Chin, J. F. S. & Whorf, T. P. Increased activity of northern vegetation inferred from atmospheric CO2 measurements. Nature 382, 146–149 (1996).

    Article  Google Scholar 

  31. Denning, A. S., Fung, I. Y. & Randall, D. Latitudinal gradient of atmospheric CO2 due to seasonal exchange with land biota. Nature 376, 240–243 (1995).

    Article  Google Scholar 

  32. Global Mercury Assessment 2013: Sources, Emissions, Releases and Environmental Transport (UNEP Chemicals Branch, Geneva, 2013).

  33. Steffen, A. et al. A synthesis of atmospheric mercury depletion event chemistry in the atmosphere and snow. Atmos. Chem. Phys. 8, 1445–1482 (2008).

    Article  Google Scholar 

  34. Diéguez, M. C. et al. Four years of atmospheric mercury records in Northwestern Patagonia (Argentina): potential sources, concentration patterns and influence of environmental variables observed at the GMOS EMMA station. Atmos. Chem. Phys. Discuss. https://doi.org/10.5194/acp-2016-1076 (2017).

  35. Fritsche, J. et al. Elemental mercury fluxes over a sub-alpine grassland determined with two micrometeorological methods. Atmos. Environ. 42, 2922–2933 (2008).

    Article  Google Scholar 

  36. Poissant, L., Pilote, M., Yumvihoze, E. & Lean, D. Mercury concentrations and foliage/atmosphere fluxes in a maple forest ecosystem in Québec, Canada. J. Geophys. Res. 113, D10307 (2008).

    Article  Google Scholar 

  37. Fu, X. et al. Depletion of atmospheric gaseous elemental mercury by plant uptake at Mt. Changbai, Northeast China. Atmos. Chem. Phys. 16, 12861–12873 (2016).

    Article  Google Scholar 

  38. Wofsy, S. C. et al. Net exchange of CO2 in a midlatitude forest. Science 260, 1314–1317 (1993).

    Article  Google Scholar 

  39. Commane, R. et al. Seasonal fluxes of carbonyl sulfide in a midlatitude forest. Proc. Natl Acad. Sci. USA 112, 14162–14167 (2015).

    Article  Google Scholar 

  40. Wehr, R. et al. Dynamics of canopy stomatal conductance, transpiration, and evaporation in a temperate deciduous forest, validated by carbonyl sulfide uptake. Biogeosciences 14, 389–401 (2017).

    Article  Google Scholar 

  41. Obrist, D. et al. A synthesis of terrestrial mercury in the western United States: spatial distribution defined by land cover and plant productivity. Sci. Total Environ. 568, 522–535 (2016).

    Article  Google Scholar 

  42. Blasing, T. J., Broniak, C. T. & Marland, G. The annual cycle of fossil-fuel carbon dioxide emissions in the United States. Tellus B 57, 107–115 (2011).

    Article  Google Scholar 

  43. Lan, X., Talbot, R., Castro, M., Perry, K. & Luke, W. Seasonal and diurnal variations of atmospheric mercury across the US determined from AMNet monitoring data. Atmos. Chem. Phys. 12, 10569–10582 (2012).

    Article  Google Scholar 

  44. Xu, X. H., Akhtar, U., Clark, K. & Wang, X. B. Temporal variability of atmospheric total gaseous mercury in Windsor, ON, Canada. Atmosphere 5, 536–556 (2014).

    Article  Google Scholar 

  45. Song, S. et al. Constraints from observations and modeling on atmosphere–surface exchange of mercury in eastern North America. Elem. Sci. Anth. 4, 100 (2016).

    Article  Google Scholar 

  46. Bieser, J. et al. in Air Pollution Modeling and its Application XXIII (eds Steyn, D. & Mathur, R.) 189–195 (Springer, Cham, 2014).

  47. Bieser, J. et al. Multi-model study of mercury dispersion in the atmosphere: vertical and interhemispheric distribution of mercury species. Atmos. Chem. Phys. 17, 6925–6955 (2017).

    Article  Google Scholar 

  48. Nemani, R. R. et al. Climate-driven increases in global terrestrial net primary production from 1982 to 1999. Science 300, 1560–1563 (2003).

    Article  Google Scholar 

  49. Zhao, M. & Running, S. W. Drought-induced reduction in global terrestrial net primary production from 2000 through 2009. Science 329, 940–943 (2010).

    Article  Google Scholar 

  50. Campbell, J. E. et al. Large historical growth in global terrestrial gross primary production. Nature 544, 84–87 (2017).

    Article  Google Scholar 

  51. Baccini, A. et al. Estimated carbon dioxide emissions from tropical deforestation improved by carbon-density maps. Nat. Clim. Change 2, 182–185 (2012).

    Article  Google Scholar 

  52. Tørseth, K. et al. Introduction to the European Monitoring and Evaluation Programme (EMEP) and observed atmospheric composition change during 1972–2009. Atmos. Chem. Phys. 12, 5447–5481 (2012).

    Article  Google Scholar 

  53. Dlugokencky, E. J., Lang, P. M., Mund, J. W., Crotwell, A. M., Crotwell, M. J. & Thoning, K. W. Atmospheric Carbon Dioxide Dry Air Mole Fractions from the NOAA ESRL Carbon Cycle Cooperative Global Air Sampling Network, 1968–2015 (NOAA, 2016); ftp://aftp.cmdl.noaa.gov/data/trace_gases/co2/flask/surface/

  54. Jiang, Y., Cizdziel, J. V. & Lu, D. Temporal patterns of atmospheric mercury species in northern Mississippi during 2011–2012: influence of sudden population swings. Chemosphere 93, 1694–1700 (2013).

    Article  Google Scholar 

  55. Lan, X. et al. Seasonal and diurnal variations of total gaseous mercury in urban Houston, TX, USA. Atmosphere 5, 399–419 (2014).

    Article  Google Scholar 

  56. Cole, A. et al. A survey of mercury in air and precipitation across Canada: patterns and trends. Atmosphere 5, 635–668 (2014).

    Article  Google Scholar 

  57. Sheu, G. R. et al. Temporal distribution and potential sources of atmospheric mercury measured at a high-elevation background station in Taiwan. Atmos. Environ. 44, 2393–2400 (2010).

    Article  Google Scholar 

  58. Zhang, L., Wang, S. X., Wang, L. & Hao, J. M. Atmospheric mercury concentration and chemical speciation at a rural site in Beijing, China: implications of mercury emission sources. Atmos. Chem. Phys. 13, 10505–10516 (2013).

    Article  Google Scholar 

  59. Read, K. A. et al. Four years (2011–2015) of total gaseous mercury measurements from the Cape Verde Atmospheric Observatory. Atmos. Chem. Phys. 17, 5393–5406 (2017).

    Article  Google Scholar 

  60. Denzler, B. et al. Inversion approach to validate mercury emissions based on background air monitoring at the High Altitude Research Station Jungfraujoch (3580 m). Environ. Sci. Technol. 51, 2846–2853 (2017).

    Article  Google Scholar 

  61. Howard, D. et al. Atmospheric mercury in the Southern Hemisphere tropics: seasonal and diurnal variations and influence of inter-hemispheric transport. Atmos. Chem. Phys. 17, 11623–11636 (2017).

    Article  Google Scholar 

  62. R Development Core Team R: A Language and Environment for Statistical Computing (R Foundation for Statistical Computing, Vienna, 2015).

  63. Liu, F. et al. High-resolution inventory of technologies, activities, and emissions of coal-fired power plants in China from 1990 to 2010. Atmos. Chem. Phys. 15, 13299–13317 (2015).

    Article  Google Scholar 

  64. Zhu, J., Wang, T., Bieser, J. & Matthias, V. Source attribution and process analysis for atmospheric mercury in eastern China simulated by CMAQ-Hg. Atmos. Chem. Phys. 15, 8767–8779 (2015).

    Article  Google Scholar 

Download references

Acknowledgements

We thank those involved in the EMEP efforts and those who have contributed by operating sites, performing chemical analysis and submitting data to the EBAS database. EMEP is funded through national contributions. We gratefully acknowledge the Air Quality Research Division of Environment Canada for the total gaseous mercury data, and the Earth System Research Laboratory at the National Oceanic and Atmospheric Administration and World Data Center for Greenhouse Gases for the CO2 data. This work contributed to the European Union 7th Framework Programme project Global Mercury Observation System. Logistical and financial support was provided by the French Polar Institute Paul-Emile Victor (Program 1028, GMOstral). This work was also funded by H2020 Marie Sklodowska-Curie grant agreement 657195 and Swiss National Science Foundation grant PZ00P2_174101 to M.J., and European Research Council grant ERC-2010-StG_20091028 to J.E.S.

Author information

Authors and Affiliations

Authors

Contributions

M.J. initiated the project, performed the data analysis and wrote the manuscript together with J.E.S. and contributions from D.O., J.B. and A.D. J.B., R.E., C.L.M., K.A.P., I.W., K.K., D.W., L.G.M., C.L., T.M., M.R., O.M. and A.D. provided data. All authors read and commented on the manuscript.

Corresponding author

Correspondence to Martin Jiskra.

Ethics declarations

Competing interests

The authors declare no competing interests.

Additional information

Publisher’s note: Springer Nature remains neutral with regard to jurisdictional claims in published maps and institutional affiliations.

Supplementary information

Supplementary Information

Supplementary Data Tables, Figures and Discussion

Rights and permissions

Reprints and permissions

About this article

Check for updates. Verify currency and authenticity via CrossMark

Cite this article

Jiskra, M., Sonke, J.E., Obrist, D. et al. A vegetation control on seasonal variations in global atmospheric mercury concentrations. Nature Geosci 11, 244–250 (2018). https://doi.org/10.1038/s41561-018-0078-8

Download citation

  • Received:

  • Accepted:

  • Published:

  • Issue Date:

  • DOI: https://doi.org/10.1038/s41561-018-0078-8

This article is cited by

Search

Quick links

Nature Briefing

Sign up for the Nature Briefing newsletter — what matters in science, free to your inbox daily.

Get the most important science stories of the day, free in your inbox. Sign up for Nature Briefing