Impact of anthropogenic atmospheric nitrogen and sulfur deposition on ocean acidification and the inorganic carbon system

  1. Scott C. Doney*,,
  2. Natalie Mahowald,
  3. Ivan Lima*,
  4. Richard A. Feely§,
  5. Fred T. Mackenzie,
  6. Jean-Francois Lamarque, and
  7. Phil J. Rasch
  1. *Marine Chemistry and Geochemistry Department, Woods Hole Oceanographic Institution, 266 Woods Hole Road, Woods Hole, MA 02543;
  2. Divisions of Climate and Global Dynamics and
  3. Atmospheric Chemistry, National Center for Atmospheric Research, 1850 Table Mesa Drive, Boulder, CO 80303;
  4. §Pacific Marine Environmental Laboratory, National Oceanic and Atmospheric Administration, 7600 Sand Point Way NE, Seattle, WA 98115-6349; and
  5. Department of Oceanography, School of Ocean and Earth Science and Technology, University of Hawaii at Manoa, 100 Pope Road, Honolulu, HI 96822
  1. Edited by Michael L. Bender, Princeton University, Princeton, NJ, and approved July 9, 2007 (received for review March 9, 2007)

Abstract

Fossil fuel combustion and agriculture result in atmospheric deposition of 0.8 Tmol/yr reactive sulfur and 2.7 Tmol/yr nitrogen to the coastal and open ocean near major source regions in North America, Europe, and South and East Asia. Atmospheric inputs of dissociation products of strong acids (HNO3 and H2SO4) and bases (NH3) alter surface seawater alkalinity, pH, and inorganic carbon storage. We quantify the biogeochemical impacts by using atmosphere and ocean models. The direct acid/base flux to the ocean is predominately acidic (reducing total alkalinity) in the temperate Northern Hemisphere and alkaline in the tropics because of ammonia inputs. However, because most of the excess ammonia is nitrified to nitrate (NO3 ) in the upper ocean, the effective net atmospheric input is acidic almost everywhere. The decrease in surface alkalinity drives a net air–sea efflux of CO2, reducing surface dissolved inorganic carbon (DIC); the alkalinity and DIC changes mostly offset each other, and the decline in surface pH is small. Additional impacts arise from nitrogen fertilization, leading to elevated primary production and biological DIC drawdown that reverses in some places the sign of the surface pH and air–sea CO2 flux perturbations. On a global scale, the alterations in surface water chemistry from anthropogenic nitrogen and sulfur deposition are a few percent of the acidification and DIC increases due to the oceanic uptake of anthropogenic CO2. However, the impacts are more substantial in coastal waters, where the ecosystem responses to ocean acidification could have the most severe implications for mankind.

Footnotes

  • To whom correspondence should be addressed. E-mail: sdoney{at}whoi.edu
  • Author contributions: S.C.D. and N.M. designed research; S.C.D., N.M., and I.L. performed research; J.-F.L. and P.J.R. contributed new reagents/analytic tools; S.C.D., N.M., and I.L. analyzed data; and S.C.D., N.M., R.A.F., and F.T.M. wrote the paper.

  • The authors declare no conflict of interest.

  • This article is a PNAS Direct Submission.

  • Abbreviations:
    Alk,
    total alkalinity;
    DIC,
    dissolved inorganic carbon.
  • Freely available online through the PNAS open access option.

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