Photochemical model performance for PM2.5 sulfate, nitrate, ammonium, and precursor species SO2, HNO3, and NH3 at background monitor locations in the central and eastern United States

被引:56
作者
Baker, Kirk
Scheff, Peter
机构
[1] Lake Michigan Air Directors Consortium, Rosemont, IL USA
[2] Univ Illinois, Chicago, IL USA
关键词
photochemical model; regional air quality; PM2.5; ammonia; nitric acid; sulfur dioxide;
D O I
10.1016/j.atmosenv.2007.04.006
中图分类号
X [环境科学、安全科学];
学科分类号
08 ; 0830 ;
摘要
Health studies have shown premature death is statistically associated with exposure to particulate matter < 2.5 mu m in diameter (PM2.5). The United States Environmental Protection Agency requires all States with PM2.5 non-attainment Counties or with sources contributing to visibility impairment at Class I areas to submit an emissions control plan. These emission control plans will likely focus on reducing emissions of sulfur oxides and nitrogen oxides, which form two of the largest chemical components of PM2.5 in the eastern United States: ammonium sulfate and ammonium nitrate. Emission control strategies are simulated using three-dimensional Eulerian photochemical transport models. A monitor study was established using one urban (Detroit) and nine rural locations in the central and eastern United (SO42-) States to simultaneously measure PM2.5 sulfate ion 4, nitrate ion (NOD, ammonium ion (NH4+), and precursor species sulfur dioxide (SO2) nitric acid (HNO3) and ammonia (NH3). This monitor study provides a unique opportunity to assess how well the modeling system predicts the spatial and temporal variability of important precursor species and co-located PM2.5 ions, which is not well characterized in the central and eastern United States. The modeling system performs well at estimating the PM2.5 species, but does not perform quite as well for the precursor species. Ammonia is under-predicted in the coldest months, nitric acid tends to be over-predicted in the summer months, and sulfur dioxide appears to be systematically over-predicted. Several indicators of PM2.5 ammonium sulfate and ammonium nitrate formation and chemical composition are estimated with the ambient data and photochemical model output. PM2.5 sulfate ion is usually not fully neutralized to ammonium sulfate in ambient measurements and is usually fully neutralized in model estimates. The model and ambient estimates agree that the ammonia study monitors tend to be nitric acid limited for PM2.5 nitrate formation. Regulatory strategies in this part of the country should focus on reductions in NOx rather than ammonia to control PM2.5 ammonium nitrate. (c) 2007 Elsevier Ltd. All rights reserved.
引用
收藏
页码:6185 / 6195
页数:11
相关论文
共 30 条
  • [21] MORRIS RE, 2004, DENV REG AIR QUAL CO
  • [22] ISORROPIA: A new thermodynamic equilibrium model for multiphase multicomponent inorganic aerosols
    Nenes, A
    Pandis, SN
    Pilinis, C
    [J]. AQUATIC GEOCHEMISTRY, 1998, 4 (01) : 123 - 152
  • [23] Influence of population density and temporal variations in emissions on the air quality benefits of NOx emission trading
    Nobel, CE
    McDonald-Butler, EC
    Kimura, Y
    Lumbley, KE
    Allen, DT
    [J]. ENVIRONMENTAL SCIENCE & TECHNOLOGY, 2002, 36 (16) : 3465 - 3473
  • [24] A temporally and spatially resolved ammonia emission inventory for dairy cows in the United States
    Pinder, RW
    Strader, R
    Davidson, CI
    Adams, PJ
    [J]. ATMOSPHERIC ENVIRONMENT, 2004, 38 (23) : 3747 - 3756
  • [25] Evaluation of secondary organic aerosol formation in winter
    Strader, R
    Lurmann, F
    Pandis, SN
    [J]. ATMOSPHERIC ENVIRONMENT, 1999, 33 (29) : 4849 - 4863
  • [26] STRADER R, 2005, CMU AMMONIA EMISSION
  • [27] Development of a chlorine mechanism for use in the carbon bond IV chemistry model
    Tanaka, PL
    Allen, DT
    McDonald-Buller, EC
    Chang, SH
    Kimura, Y
    Mullins, CB
    Yarwood, G
    Neece, JD
    [J]. JOURNAL OF GEOPHYSICAL RESEARCH-ATMOSPHERES, 2003, 108 (D4)
  • [28] Use of two different acidic aerosol samplers to measure acidic aerosols in Hsinchu, Taiwan
    Tsai, CJ
    Perng, SB
    Chiou, SF
    [J]. JOURNAL OF THE AIR & WASTE MANAGEMENT ASSOCIATION, 2000, 50 (12): : 2120 - 2128
  • [29] *US EPA, 2006, GUID US MOD AN DEM A
  • [30] WILKINSON JG, 1994, SARMAP LMOS EMISSION