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.

  • Letter
  • Published:

Dissolved organic carbon trends resulting from changes in atmospheric deposition chemistry

Abstract

Several hypotheses have been proposed to explain recent, widespread increases in concentrations of dissolved organic carbon (DOC) in the surface waters of glaciated landscapes across eastern North America and northern and central Europe1,2,3. Some invoke anthropogenic forcing through mechanisms related to climate change3,4,5, nitrogen deposition6 or changes in land use7, and by implication suggest that current concentrations and fluxes are without precedent. All of these hypotheses imply that DOC levels will continue to rise, with unpredictable consequences for the global carbon cycle. Alternatively, it has been proposed that DOC concentrations are returning toward pre-industrial levels as a result of a gradual decline in the sulphate content of atmospheric deposition8,9,10. Here we show, through the assessment of time series data from 522 remote lakes and streams in North America and northern Europe, that rising trends in DOC between 1990 and 2004 can be concisely explained by a simple model based solely on changes in deposition chemistry and catchment acid-sensitivity. We demonstrate that DOC concentrations have increased in proportion to the rates at which atmospherically deposited anthropogenic sulphur and sea salt have declined. We conclude that acid deposition to these ecosystems has been partially buffered by changes in organic acidity and that the rise in DOC is integral to recovery from acidification. Over recent decades, deposition-driven increases in organic matter solubility may have increased the export of DOC to the oceans, a potentially important component of regional carbon balances11. The increase in DOC concentrations in these regions appears unrelated to other climatic factors.

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

Figure 1: Trends in dissolved organic carbon (mg l-1 yr-1).
Figure 2: Relationship between %ΔDOC, ΔSO 4 2- and ΔCl - and the equivalent sum of ΔSO 4 2- and ΔCl - , used as surrogates for changes in atmospheric deposition.
Figure 3: Distributions of %ΔDOC and residuals from multiple regression, by region.

Similar content being viewed by others

References

  1. Roulet, N. & Moore, T. R. Browning the waters. Nature 444, 283–284 (2006)

    Article  ADS  CAS  Google Scholar 

  2. Skjelkvåle, B. L. et al. Regional scale evidence for improvements in surface water chemistry 1990–2001. Environ. Pollut. 137, 165–176 (2005)

    Article  Google Scholar 

  3. Worrall, F., Burt, T. & Shedden, R. Long term records of riverine dissolved organic matter. Biogeochemistry 64, 165–178 (2003)

    Article  CAS  Google Scholar 

  4. Freeman, C., Evans, C. D., Monteith, D. T., Reynolds, B. & Fenner, N. Export of organic carbon from peat soils. Nature 412, 785 (2001)

    Article  ADS  CAS  Google Scholar 

  5. Freeman, C. et al. Export of dissolved organic carbon from peatlands under elevated carbon dioxide levels. Nature 430, 195–198 (2004)

    Article  ADS  CAS  Google Scholar 

  6. Findlay, S. E. G. Increased carbon transport in the Hudson River: unexpected consequence of nitrogen deposition? Frontiers Ecol. Environ. 3, 133–137 (2005)

    Article  Google Scholar 

  7. Garnett, M. H., Ineson, P. & Stevenson, A. C. Effects of burning and grazing on carbon sequestration in a Pennine blanket bog. Holocene 10, 729–736 (2000)

    Article  ADS  Google Scholar 

  8. Evans, C. D., Chapman, P. J., Clark, J. M., Monteith, D. T. & Cresser, M. S. Alternative explanations for rising dissolved organic carbon export from organic soils. Glob. Change Biol. 12, 1–10 (2006)

    Article  Google Scholar 

  9. Stoddard, J. L. et al. Response of Surface Water Chemistry to the Clean Air Act Amendments of 1990. Report EPA/620/R-03/001 (US Environmental Protection Agency, Washington DC, 2003)

    Google Scholar 

  10. Vuorenmaa, J., Forsius, M. & Mannio, J. Increasing trends of total organic carbon concentrations in small forest lakes in Finland from 1987 to 2003. Sci. Total Environ. 365, 47–65 (2006)

    Article  ADS  CAS  Google Scholar 

  11. Siemens, J. The European carbon budget: a gap. Science 302, 1681 (2003)

    Article  CAS  Google Scholar 

  12. Evans, C. D. & Monteith, D. T. Chemical trends at lakes and streams in the UK Acid Waters Monitoring Network, 1988–2000: Evidence for recent recovery at a national scale. Hydrol. Earth Syst. Sci. 5, 351–366 (2001)

    Article  ADS  Google Scholar 

  13. Alewell, C., Mitchell, M. J., Likens, G. E. & Krouse, H. R. Sources of stream sulfate at the Hubbard Brook Experimental Forest. Biogeochemistry 44, 281–299 (1999)

    Google Scholar 

  14. Tranvik, I. J. & Jansson, M. Terrestrial export of organic carbon. Nature 415, 861–862 (2002)

    Article  ADS  CAS  Google Scholar 

  15. Hejzlar, J., Dubrovsky, M., Buchtele, J. & Ruzicka, M. The apparent and potential effects of climate change on the inferred concentration of dissolved organic matter in a temperate stream (the Malse River, South Bohemia). Sci. Total Environ. 310, 142–152 (2003)

    Article  ADS  Google Scholar 

  16. Evans, C. D., Monteith, D. T. & Cooper, D. M. Long-term increases in surface water dissolved organic carbon: Observations, possible causes and environmental impacts. Environ. Pollut. 137, 55–71 (2005)

    Article  CAS  Google Scholar 

  17. Zhu, Y. & Day, R. L. Analysis of streamflow trends and the effects of climate in Pennsylvania, 1971 to 2001. J. Am. Water Resour. Assoc. 41, 1393–1405 (2005)

    Article  ADS  Google Scholar 

  18. de Wit, H. A., Hindar, A. & Hole, L. Winter climate affects long-term trends in stream water nitrate in acid-sensitive catchments in southern Norway. Hydrol. Earth Syst. Sci. 4, 3055–3085 (2007)

    Article  Google Scholar 

  19. Whitfield, P. H. & Cannon, A. J. Recent variations in climate and hydrology in Canada. Can. Water Resour. J. 25, 19–65 (2000)

    Article  Google Scholar 

  20. Hyvärinen, V. Trends and characteristics of hydrological time series in Finland. Nordic Hydrol. 34, 71–90 (2003)

    Article  Google Scholar 

  21. Wright, R. F. et al. Trends in nitrogen deposition and leaching in acid-sensitive streams in Europe. Hydrol. Earth Syst. Sci. 5, 299–310 (2001)

    Article  ADS  Google Scholar 

  22. Krug, E. C. & Frink, C. R. Acid rain on acid soil: a new perspective. Science 221, 520–525 (1983)

    Article  ADS  CAS  Google Scholar 

  23. Clark, J. M., Chapman, P. J., Heathwaite, A. L. & Adamson, J. K. Suppression of dissolved organic carbon by sulphate induced acidification during simulated droughts. Environ. Sci. Technol. 40, 1776–1783 (2006)

    Article  ADS  CAS  Google Scholar 

  24. de Wit, H. A., Groseth, T. & Mulder, J. Predicting aluminum and soil organic matter solubility using the mechanistic equilibrium model WHAM. Soil Sci. Soc. Am. J. 65, 1089–1100 (2001)

    Article  ADS  CAS  Google Scholar 

  25. Vogt, R. D., Ranneklev, S. B. & Mykkelbost, T. C. The impact of acid treatment on soilwater chemistry at the HUMEX site. Environ. Int. 3, 277–286 (1994)

    Article  Google Scholar 

  26. Tipping, E. & Hurley, M. A. A model of solid-solution interactions in acid organic soils, based on the complexation properties of humic substances. J. Soil Sci. 39, 505–519 (1988)

    Article  CAS  Google Scholar 

  27. Tipping, E. & Woof, C. The distribution of humic substances between the solid and aqueous phases of acid organic soils; a description based on humic heterogeneity and charge-dependent sorption equilibria. J. Soil Sci. 42, 437–448 (1991)

    Article  CAS  Google Scholar 

  28. Evans, A., Zelazny, L. W. & Zipper, C. E. Solution parameters influencing dissolved organic carbon levels in three forest soils. Soil Sci. Soc. Am. J. 52, 1789–1792 (1988)

    Article  ADS  CAS  Google Scholar 

  29. Sokal, R. R. & Rohlf, F. J. Biometry 532–538 (W. H. Freeman, San Francisco, 1969)

    MATH  Google Scholar 

  30. Sen, P. K. On a class of aligned rank order tests in two-way layouts. Ann. Math. Stat. 39, 1115–1124 (1968)

    Article  MathSciNet  Google Scholar 

Download references

Acknowledgements

We thank the LRTAP Working Group on Effects and the EU 6th Framework Programme Euro-limpacs for support in the production and analysis of international, quality-controlled, comparable data. We also acknowledge the work of the ICP Waters Programme Centre at the Norwegian Institute of Water Research (NIVA), where the data were collated, verified and archived. The authors are indebted to many colleagues and organisations who provided data for this assessment, including: T. A. Clair, S. Couture, C. Gagnon, D. K. McNicol, R. C. Weeber, A. Paterson (Canada); J. S. Kahl, J. Kellogg, K. Roy, M. R. Hale, D. R. DeWalle (USA); the Finnish Environment Institute (SYKE) and Regional Environment Centres; the Norwegian Institute of Water Research (NIVA); the Swedish Environmental Protection Agency (Naturvårdsverket); and the UK Acid Waters Monitoring Network (supported by the Department for Environment Food and Rural Affairs) and supporting laboratories at: Fisheries Research Services, Pitlochry; Centre for Ecology and Hydrology, Wallingford; and the Environment Agency Llanelli. The information in this document has been funded in part by the US Environmental Protection Agency. It has been subjected to review by the National Health and Environmental Effects Research Laboratory, and approved for publication. Approval does not signify that the contents reflect the views of the Agency, nor does mention of trade names or commercial products constitute endorsement or recommendation for use.

Author Contributions D.T.M. and J.L.S. formulated the working hypothesis and analysed and interpreted the trend data. C.D.E. and H.A.d.W. contributed to the development of the hypothesis, assisted in the interpretation of the data, provided additional text and edited the manuscript. M.F., T.H., A.W., B.L.S., D.S.J., B.K. and J. Vuorenmaa provided data and commented on the text. J.K. provided advice and ideas on processes and contributed data from the Czech Republic (not included in the final analysis due to number and length of time series) consistent with the hypothesis. J. Vesely contributed advice, ideas and data in the early stages of development of our work.

Author information

Authors and Affiliations

Authors

Corresponding author

Correspondence to Donald T. Monteith.

Supplementary information

Supplementary Information

The file contains Supplementary Figures S1-S3 and Supplementary Tables S1-S5 with Legends. (PDF 744 kb)

Rights and permissions

Reprints and permissions

About this article

Cite this article

Monteith, D., Stoddard, J., Evans, C. et al. Dissolved organic carbon trends resulting from changes in atmospheric deposition chemistry. Nature 450, 537–540 (2007). https://doi.org/10.1038/nature06316

Download citation

  • Received:

  • Accepted:

  • Issue Date:

  • DOI: https://doi.org/10.1038/nature06316

This article is cited by

Comments

By submitting a comment you agree to abide by our Terms and Community Guidelines. If you find something abusive or that does not comply with our terms or guidelines please flag it as inappropriate.

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