References

ACPD

Atmospheric Chemistry and Physics Discussions

ACPD

Atmos. Chem. Phys. Discuss.

1680-7375

Göttingen, Germany

10.5194/acpd-10-28183-2010

The impact of different nitrous acid sources in the air quality levels of the Iberian Peninsula

Gonçalves

¹ ² Dabdub

³ Chang

W. L.

³ Saiz

³ Jorba

² Baldasano

J. M.

¹ ²

Environmental Modeling Laboratory, Projects Department, Technical University of Catalonia, Barcelona, Spain

Earth Sciences Department, Barcelona Supercomputing Center, Barcelona, Spain

Department of Mechanical and Aerospace Engineering, University of California, Irvine, Irvine, California, USA

17 11 2010

10 11 28183 28230

2010

This work is licensed under the Creative Commons Attribution 3.0 Unported License. To view a copy of this licence, visit https://creativecommons.org/licenses/by/3.0/

This article is available from https://acp.copernicus.org/preprints/10/28183/2010/acpd-10-28183-2010.html

The full text article is available as a PDF file from https://acp.copernicus.org/preprints/10/28183/2010/acpd-10-28183-2010.pdf

Hydroxyl radical (OH) is a primary oxidant in the atmosphere and affects both gas-phase pollutants and particulate matter levels. Nitrous acid (HONO) acts as an important source of OH in the urban atmosphere. Therefore it is important to account accurately for HONO sources within air quality models in order to predict air pollution dynamics. HONO observations in urban areas are characterized by high concentrations at night and low concentrations around midday. Existing gas-phase chemical mechanisms do not reproduce the observed HONO levels, suggesting a lack of sources, such as direct emissions or heterogeneous reactions. Specific HONO emission rates, heterogeneous chemical mechanisms leading to its formation and related kinetics are still unclear. Therefore, most air quality models consider exclusively gas-phase chemistry related to HONO. This work applies the WRF-ARW/HERMES/CMAQ modeling system to quantify the effect of the addition of HONO sources in the predictability of HONO profiles, and its subsequent effect on secondary pollutants formation (mainly O3 and PM2.5). The modeling episode is based on a 2004 severe summertime pollution event in the Iberian Peninsula, using high resolution of 4 × 4 km2. Two different parameterizations for emissions and the hydrolysis of NO2 on wet surfaces are added as HONO sources in the atmosphere. Emissions have the largest impact on HONO levels, especially in urban areas, where they can contribute from 66% to 94% to the HONO peak concentration. Additionally, in urban environments, NO2 hydrolysis on building and vegetation surfaces contributes up to 30% to the HONO peak. Both, the available surface area and the relative humidity must be included as parameters affecting the NO2 hydrolysis kinetics. As a result, NO2 hydrolysis is negligible on aerosol surfaces, due to the small surface area available for reaction, and it is more effective in producing HONO below high relative humidity conditions. The addition of HONO sources affects the concentration of secondary pollutants. In particular, major changes are produced in the early morning, due to the higher OH release via HONO photolysis. Significant changes in PM2.5 concentrations are predicted, that can be 16% (2.6 μg m−3) higher in the new scenarios. When accounting for HONO sources, nitrate levels increase especially in urban areas and sulfates in areas downwind from conventional power plants in the Iberian Peninsula. Also, O3 peak concentrations are slightly affected (from 0.7 to 4 ppb, 1% to 4.5%). The improvement of the HONO sources representation within air quality models produces changes in O3 peak predictions and significantly affects the reaction pathways leading to aerosols formation. Therefore, HONO sources other than gas-phase chemistry should be accurately included within modeling frameworks.

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