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Size distribution of sea-salt emissions as a function of relative humidity (2005)

ZHANG, K ; KNIPPING, E ; WEXLER, A ; [et al.]

Elsevier

In: Atmospheric Environment. 2005; 39(18): 3373-3379. Published 2005 Jun 01. doi: 10.1016/j.atmosenv.2005.02.032.

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Publication Date: 2005-06-01

Print ISSN: 1352-2310

Electronic ISSN: 1873-2844

Topics: Energy, Environment Protection, Nuclear Power Engineering , Geosciences , Physics

Published by Elsevier

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Modeling urban and regional aerosols—Application of the CMAQ-UCD Aerosol Model to Tampa, a coastal urban site (2008)

NOLTE, C ; BHAVE, P ; ARNOLD, J ; [et al.]

Elsevier

In: Atmospheric Environment. 2008; 42(13): 3179-3191. Published 2008 Apr 01. doi: 10.1016/j.atmosenv.2007.12.059.

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Publication Date: 2008-04-01

Print ISSN: 1352-2310

Electronic ISSN: 1873-2844

Topics: Energy, Environment Protection, Nuclear Power Engineering , Geosciences , Physics

Published by Elsevier

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Examining the impact of heterogeneous nitryl chloride production on air quality across the United States (2012)

Sarwar, G. ; Simon, H. ; Bhave, P. ; [et al.]

Copernicus

In: Atmospheric Chemistry and Physics Discussions. 2012; 12(2): 6145-6183. Published 2012 Feb 27. doi: 10.5194/acpd-12-6145-2012.

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Publication Date: 2012-02-27

Description: The heterogeneous hydrolysis of dinitrogen pentoxide (N2O5) has typically been modeled as only producing nitric acid. However, recent field studies have confirmed that the presence of particulate chloride alters the reaction product to produce nitryl chloride (ClNO2) which undergoes photolysis to generate chlorine atoms and nitrogen dioxide (NO2). Both chlorine and NO2 affect atmospheric chemistry and air quality. We present an updated gas-phase chlorine mechanism that can be combined with the Carbon Bond 05 mechanism and incorporate the combined mechanism into the Community Multiscale Air Quality modeling system. We then update the current model treatment of heterogeneous hydrolysis of N2O5 to include ClNO2 as a product. The model, in combination with a comprehensive inventory of chlorine compounds, reactive nitrogen, particulate matter, and organic compounds, is used to evaluate the impact of the heterogeneous ClNO2 production on air quality across the United States for the months of February and September in 2006. The heterogeneous production increases ClNO2 in coastal as well as many in-land areas in the United States. Particulate chloride derived from sea-salts, anthropogenic sources, and forest fires activates the heterogeneous production of ClNO2. With current estimates of tropospheric emissions burden, it modestly enhances monthly mean 8-h ozone (up to 1–2 ppbv or 3–4%) but causes large increases (up to 13 ppbv) in isolated episodes. It also substantially reduce the mean total nitrate by up to 0.8–2.0 μg m−3 or 11–21%. Modeled ClNO2 accounts for up to 3–4% of the monthly mean total reactive nitrogen. Sensitivity results of the model suggest that ClNO2 formation is limited more by the presence of particulate chloride than by the abundance of N2O5.

Electronic ISSN: 1680-7375

Topics: Geosciences

Published by Copernicus on behalf of European Geosciences Union.

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Determining the spatial and seasonal variability in OM/OC ratios across the US using multiple regression (2010)

Simon, H. ; Bhave, P. V. ; Swall, J. L. ; [et al.]

Copernicus

In: Atmospheric Chemistry and Physics Discussions. 2010; 10(10): 24651-24698. Published 2010 Oct 21. doi: 10.5194/acpd-10-24651-2010.

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Publication Date: 2010-10-21

Description: Data from the Interagency Monitoring of Protected Visual Environments (IMPROVE) network are used to estimate organic mass to organic carbon (OM/OC) ratios across the United States by extending previously published multiple regression techniques. Our new methodology addresses common pitfalls of multiple regression including measurement uncertainty, colinearity of covariates, and dataset selection. As expected, summertime OM/OC ratios are larger than wintertime values across the US with all regional median OM/OC values tightly confined between 1.8 and 1.95. Further, we find that OM/OC ratios during the winter are distinctly larger in the eastern US than in the West (regional medians are 1.58, 1.64, and 1.85 in the great lakes, southeast, and northeast regions, versus 1.29 and 1.32 in the western and central states). We find less spatial variability in long-term averaged OM/OC ratios across the US (90% of our multiyear regressions predicted OM/OC ratios between 1.37 and 1.94) than previous studies (90% of OM/OC estimates from a previous regression study fell between 1.30 and 2.10). We attribute this difference largely to the inclusion of EC as a covariate in previous regression studies. Due to the colinearity of EC and OC, we believe that up to one-quarter of the OM/OC estimates in a previous study are biased low. In addition to estimating OM/OC ratios, our technique reveals trends that may be contrasted with conventional assumptions regarding nitrate, sulfate, and soil across the IMPROVE network. For example, our regressions show pronounced seasonal and spatial variability in both nitrate volatilization and sulfate neutralization and hydration.

Electronic ISSN: 1680-7375

Topics: Geosciences

Published by Copernicus on behalf of European Geosciences Union.

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Parameterization of N2O5 reaction probabilities on the surface of particles containing ammonium, sulfate, and nitrate (2007)

Davis, J. M. ; Bhave, P. V. ; Foley, K. M.

Copernicus

In: Atmospheric Chemistry and Physics Discussions. 2007; 7(6): 16119-16153. Published 2007 Nov 19. doi: 10.5194/acpd-7-16119-2007.

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Publication Date: 2007-11-19

Description: A comprehensive parameterization was developed for the heterogeneous reaction probability (γ) of N2O5 as a function of temperature, relative humidity, particle composition, and phase state, for use in advanced air quality models. The reaction probabilities on aqueous NH4HSO4, (NH4)2SO4, and NH4NO3 were modeled statistically using data and uncertainty values compiled from seven different laboratory studies. A separate regression model was fit to laboratory data for dry NH4HSO4 and (NH4)2SO4 particles, yielding lower γ values than the corresponding aqueous parameterizations. The regression equations reproduced 79% of the laboratory data within a factor of two and 53% within a factor of 1.25. A fixed value was selected for γ on ice-containing particles based on a review of the literature. The combined parameterization was applied under atmospheric conditions representative of the eastern United States using 3-dimensional fields of temperature, relative humidity, sulfate, nitrate, and ammonium, obtained from a recent Community Multiscale Air Quality model simulation. The resulting spatial distributions of γ were contrasted with three other parameterizations that have been applied in air quality models in the past and with atmospheric observational determinations of γ. Our results highlight a critical need for more laboratory measurements of γ at low temperature and high relative humidity to improve model simulations of N2O5 hydrolysis during wintertime conditions.

Electronic ISSN: 1680-7375

Topics: Geosciences

Published by Copernicus on behalf of European Geosciences Union.

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