Citation:

Zhang, Y., R. Mathur, J. Bash, C. Hogrefe, J. Xing, AND S. Roselle. Long-term trends in total inorganic nitrogen and sulfur deposition in the US from 1990 to 2010. Atmospheric Chemistry and Physics. Copernicus Publications, Katlenburg-Lindau, Germany, 18:9091-9106, (2018). https://doi.org/10.5194/acp-18-9091-2018

Impact/Purpose:

Analysis of model estimates of wet and dry deposition of various atmospheric constituents across the U.S. for the 1990-2010 period show significant reductions in atmospheric deposition of sulfur and nitrogen to terrestrial and aquatic ecosystems across the U.S. and these are attributed to reductions in emissions of SO2 and NOx during this period. Though the amount of oxidized-N deposition has reduced during the period in response to NOx emission reductions, a significant increase in reduced-N deposition is seen due to increase in NH3 emissions from livestock farming. This increase in reduced-N deposition is dominated by increasing amounts of NH3 dry deposited. Reductions in SO2 and NOx emissions (and consequently their oxidation products) have decreased the amounts of NHx partitioning to the aerosol phase where scavenging by rain is the primary sink. Consequently, more NHx remains in the gas-phase and dry deposits closer to the source regions. These results reinforce the need for more extensive measurements to characterize bi-directional land-atmosphere exchange of NH3 to better constrain model calculations.

Description:

Excess deposition (including both wet and dry deposition) of nitrogen and sulfur are detrimental to ecosystems. Recent studies have investigated the spatial patterns and temporal trends of nitrogen and sulfur wet deposition, but few studies have focused on dry deposition due to the scarcity of dry deposition measurements. Here, we use long-term model simulations from the coupled WRF-CMAQ model covering the period from 1990 to 2010 to study changes in spatial distribution as well as temporal trends in total (TDEP), wet (WDEP) and dry deposition (DDEP) of total inorganic nitrogen (TIN) and sulfur (TSO4). We first evaluate the model’s performance in simulating WDEP over the U.S. by comparing the model results with observational data from the U.S. National Atmospheric Deposition Program. The coupled model generally underestimates the WDEP of both TIN (including both the oxidized nitrogen deposition-TNO3, and the reduced nitrogen deposition-NHX) and TSO4, with better performance in the eastern U.S. than the western U.S. TDEP of both TIN and TSO4 show significant decreases over the U.S., especially in the east due to the large emission reductions that occurred in that region. The decreasing trends of TIN TDEP are caused by decrease of TNO3, and the increasing trends of TIN deposition over the Great Plains and Tropical Wet Forests regions are caused by increases in NH3 emissions although it should be noted that these increasing trends are not significant. TIN WDEP shows decreasing trends throughout the U.S., except for the Marine West Coast Forest region. TIN DDEP shows significant decreasing trends in the region of Eastern Temperate Forests, Northern Forests, Mediterranean California and Marine West Coast Forest, and significant increasing trends in the region of Tropical Wet Forests, Great Plains and Southern Semi-arid Highlands. For the other three regions (North American Deserts, Temperate Sierras and Northwestern Forested Mountains), the decreasing or increasing trends were not significant. Both the WDEP and DDEP of TSOx have decreases across the U.S., with a larger decreasing trend in the DDEP than that in the WDEP. Across the U.S. during the 1990-2010 period, DDEP of TIN accounted for 58-65% of TDEP of TIN. TDEP of TIN over the U.S. was dominated by deposition of TNO3 during the first decade, which then shifts to reduced nitrogen (NHX) dominance after 2003 resulting from combination of NOx emission reductions and NH3 emission increases. The sulfur DDEP is usually higher than the sulfur WDEP until recent years, as the sulfur DDEP has a larger decreasing trend than WDEP.

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