Inverse modeling and mapping US air quality influences of inorganic PM<sub>2.5</sub> precursor emissions using the adjoint of GEOS-Chem
-
Published:2009-08-19
Issue:16
Volume:9
Page:5877-5903
-
ISSN:1680-7324
-
Container-title:Atmospheric Chemistry and Physics
-
language:en
-
Short-container-title:Atmos. Chem. Phys.
Author:
Henze D. K.,Seinfeld J. H.,Shindell D. T.
Abstract
Abstract. Influences of specific sources of inorganic PM2.5 on peak and ambient aerosol concentrations in the US are evaluated using a combination of inverse modeling and sensitivity analysis. First, sulfate and nitrate aerosol measurements from the IMPROVE network are assimilated using the four-dimensional variational (4D-Var) method into the GEOS-Chem chemical transport model in order to constrain emissions estimates in four separate month-long inversions (one per season). Of the precursor emissions, these observations primarily constrain ammonia (NH3). While the net result is a decrease in estimated US~NH3 emissions relative to the original inventory, there is considerable variability in adjustments made to NH3 emissions in different locations, seasons and source sectors, such as focused decreases in the midwest during July, broad decreases throughout the US~in January, increases in eastern coastal areas in April, and an effective redistribution of emissions from natural to anthropogenic sources. Implementing these constrained emissions, the adjoint model is applied to quantify the influences of emissions on representative PM2.5 air quality metrics within the US. The resulting sensitivity maps display a wide range of spatial, sectoral and seasonal variability in the susceptibility of the air quality metrics to absolute emissions changes and the effectiveness of incremental emissions controls of specific source sectors. NH3 emissions near sources of sulfur oxides (SOx) are estimated to most influence peak inorganic PM2.5 levels in the East; thus, the most effective controls of NH3 emissions are often disjoint from locations of peak NH3 emissions. Controls of emissions from industrial sectors of SOx and NOx are estimated to be more effective than surface emissions, and changes to NH3 emissions in regions dominated by natural sources are disproportionately more effective than regions dominated by anthropogenic sources. NOx controls are most effective in northern states in October; in January, SOx controls may be counterproductive. When considering ambient inorganic PM2.5 concentrations, intercontinental influences are small, though transboundary influences within North America are significant, with SOx emissions from surface sources in Mexico contributing almost a fourth of the total influence from this sector.
Publisher
Copernicus GmbH
Subject
Atmospheric Science
Reference115 articles.
1. Adams, P J., Seinfeld, J H., and Koch, D M.: Global concentrations of tropospheric sulfate, nitrate, and ammonium aerosol simulated in a general circulation model, J. Geophys. Res.-Atmos., 104, 13791–13823, 1999. 2. Alexander, B., Park, R J., Jacob, D J., Li, Q B., Yantosca, R M., Savarino, J., Lee, C C. W., and Thiemens, M H.: Sulfate formation in sea-salt aerosols: Constraints from oxygen isotopes, J. Geophys. Res.-Atmos., 110, D10307, https://doi.org/10.1029/2004JD005659, 2005. 3. Baumgardner, R E., Lavery, T F., Rogers, C M., and Isil, S S.: Estimates of the atmospheric deposition of sulfur and nitrogen species: Clean Air Status and Trends Network, 1990–2000, Environ. Sci. Technol., 36, 2614–2629, 2002. 4. Beer, R., Shephard, M W., Kulawik, S., Clough, S A., Eldred, R A., Bowman, K W., Sander, S P., Fisher, B M., Payne, V H., Louo, M., Osterman, G B., and Worden, J R.: First satellite observations of lower tropospheric ammonia and methanol, Geophys. Res. Lett., 35, L09801, \\doi10.1029/2008GL033642, 2008. 5. Benkovitz, C M., Scholtz, M T., Pacyna, J., Tarrason, L., Dignon, J., Voldner, E C., Spiro, P A., Logan, J A., and Graedel, T E.: Global gridded inventories of anthropogenic emissions of sulfur and nitrogen, J. Geophys. Res.-Atmos., 101, 29239–29253, 1996.
Cited by
208 articles.
订阅此论文施引文献
订阅此论文施引文献,注册后可以免费订阅5篇论文的施引文献,订阅后可以查看论文全部施引文献
|
|