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Past, Present, and Future Atmospheric Nitrogen Deposition

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  • 1 Environmental Chemical Processes Laboratory, Department of Chemistry, University of Crete, Heraklion, Greece
  • 2 School of Earth and Atmospheric Sciences, and School of Chemical and Biomolecular Engineering, Georgia Institute of Technology, Atlanta, Georgia
  • 3 Centre for Ocean and Atmospheric Sciences, School of Environmental Sciences, University of East Anglia, Norwich, United Kingdom
  • 4 Center for Climate Systems Research, Columbia University, and NASA Goddard Institute for Space Studies, New York, New York
  • 5 Environmental Chemical Processes Laboratory, Department of Chemistry, University of Crete, Heraklion, and Institute for Environmental Research and Sustainable Development, National Observatory of Athens, Athens, Greece
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Abstract

Reactive nitrogen emissions into the atmosphere are increasing as a result of human activities, affecting nitrogen deposition to the surface and impacting the productivity of terrestrial and marine ecosystems. An atmospheric chemistry–transport model [Tracer Model 4 of the Environmental Chemical Processes Laboratory (TM4-ECPL)] is here used to calculate the global distribution of total nitrogen deposition, accounting for the first time for both its inorganic and organic fractions in gaseous and particulate phases and past and projected changes due to anthropogenic activities. The anthropogenic and biomass-burning Atmospheric Chemistry and Climate Model Intercomparison Project (ACCMIP) historical and RCP6.0 and RCP8.5 emissions scenarios are used. Accounting for organic nitrogen (ON) primary emissions, the present-day global nitrogen atmospheric source is about 60% anthropogenic, while total N deposition increases by about 20% relative to simulations without ON primary emissions. About 20%–25% of total deposited N is ON. About 10% of the emitted nitrogen oxides are deposited as ON instead of inorganic nitrogen (IN), as is considered in most global models. Almost a threefold increase over land (twofold over the ocean) has been calculated for soluble N deposition due to human activities from 1850 to present. The investigated projections indicate significant changes in the regional distribution of N deposition and chemical composition, with reduced compounds gaining importance relative to oxidized ones, but very small changes in the global total flux. Sensitivity simulations quantify uncertainties due to the investigated model parameterizations of IN partitioning onto aerosols and of N chemically fixed on organics to be within 10% for the total soluble N deposition and between 25% and 35% for the dissolved ON deposition. Larger uncertainties are associated with N emissions.

Supplemental information related to this paper is available at the Journals Online website: http://dx.doi.org/10.1175/JAS-D-15-0278.s1.

Current affiliation: LATMOS, IPSL, Paris, France.

Corresponding author address: M. Kanakidou, Environmental Chemical Processes Laboratory, Department of Chemistry, University of Crete, Voutes Campus, P.O. Box 2208, 70013 Heraklion, Greece. E-mail: mariak@uoc.gr

Abstract

Reactive nitrogen emissions into the atmosphere are increasing as a result of human activities, affecting nitrogen deposition to the surface and impacting the productivity of terrestrial and marine ecosystems. An atmospheric chemistry–transport model [Tracer Model 4 of the Environmental Chemical Processes Laboratory (TM4-ECPL)] is here used to calculate the global distribution of total nitrogen deposition, accounting for the first time for both its inorganic and organic fractions in gaseous and particulate phases and past and projected changes due to anthropogenic activities. The anthropogenic and biomass-burning Atmospheric Chemistry and Climate Model Intercomparison Project (ACCMIP) historical and RCP6.0 and RCP8.5 emissions scenarios are used. Accounting for organic nitrogen (ON) primary emissions, the present-day global nitrogen atmospheric source is about 60% anthropogenic, while total N deposition increases by about 20% relative to simulations without ON primary emissions. About 20%–25% of total deposited N is ON. About 10% of the emitted nitrogen oxides are deposited as ON instead of inorganic nitrogen (IN), as is considered in most global models. Almost a threefold increase over land (twofold over the ocean) has been calculated for soluble N deposition due to human activities from 1850 to present. The investigated projections indicate significant changes in the regional distribution of N deposition and chemical composition, with reduced compounds gaining importance relative to oxidized ones, but very small changes in the global total flux. Sensitivity simulations quantify uncertainties due to the investigated model parameterizations of IN partitioning onto aerosols and of N chemically fixed on organics to be within 10% for the total soluble N deposition and between 25% and 35% for the dissolved ON deposition. Larger uncertainties are associated with N emissions.

Supplemental information related to this paper is available at the Journals Online website: http://dx.doi.org/10.1175/JAS-D-15-0278.s1.

Current affiliation: LATMOS, IPSL, Paris, France.

Corresponding author address: M. Kanakidou, Environmental Chemical Processes Laboratory, Department of Chemistry, University of Crete, Voutes Campus, P.O. Box 2208, 70013 Heraklion, Greece. E-mail: mariak@uoc.gr
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