Maria. Teresa Pay

An annual assessment of air quality with the CALIOPE modeling system over Spain.

The CALIOPE project, funded by the Spanish Ministry of the Environment, aims at establishing an air quality forecasting system for Spain. With this goal, CALIOPE modeling system was developed and applied with high resolution (4km×4km, 1h) using the HERMES emission model (including emissions of resuspended particles from paved roads) specifically built up for Spain. The present study provides an evaluation and the assessment of the modeling system, coupling WRF-ARW/HERMES/CMAQ/BSC-DREAM8b for a full-year simulation in 2004 over Spain. The evaluation focuses on the capability of the model to reproduce the temporal and spatial distribution of gas phase species (NO(2), O(3), and SO(2)) and particulate matter (PM10) against ground-based measurements from the Spanish air quality monitoring network. The evaluation of the modeling results on an hourly basis shows a strong dependency of the performance of the model on the type of environment (urban, suburban and rural) and the dominant emission sources (traffic, industrial, and background). The O(3) chemistry is best represented in summer, when mean hourly variability and high peaks are generally well reproduced. The mean normalized error and bias meet the recommendations proposed by the United States Environmental Protection Agency (US-EPA) and the European regulations. Modeled O(3) shows higher performance for urban than for rural stations, especially at traffic stations in large cities, since stations influenced by traffic emissions (i.e., high-NO(x) environments) are better characterized with a more pronounced daily variability. NO(x)/O(3) chemistry is better represented under non-limited-NO(2) regimes. SO(2) is mainly produced from isolated point sources (power generation and transformation industries) which generate large plumes of high SO(2) concentration affecting the air quality on a local to national scale where the meteorological pattern is crucial. The contribution of mineral dust from the Sahara desert through the BSC-DREAM8b model helps to satisfactorily reproduce episodic high PM10 concentration peaks at background stations. The model assessment indicates that one of the main air quality-related problems in Spain is the high level of O(3). A quarter of the Iberian Peninsula shows more than 30days exceeding the value 120μgm(-3) for the maximum 8-h O(3) concentration as a consequence of the transport of O(3) precursors downwind to/from the Madrid and Barcelona metropolitan areas, and industrial areas and cities in the Mediterranean coast.

Assessment of Kalman filter bias-adjustment technique to improve the simulation of ground-level ozone over Spain

The CALIOPE air quality modelling system has been used to diagnose ground level O(3) concentration for the year 2004, over the Iberian Peninsula. We investigate the improvement in the simulation of daily O(3) maximum by the use of a post-processing such as the Kalman filter bias-adjustment technique. The Kalman filter bias-adjustment technique is a recursive algorithm to optimally estimate bias-adjustment terms from previous measurements and model results. The bias-adjustment technique improved the simulation of daily O(3) maximum for the entire year and the all the stations considered over the whole domain. The corrected simulation presents improvements in statistical indicators such as correlation, root mean square error, mean bias, and gross error. After the post-processing the exceedances of O(3) concentration limits, as established by the European Directive 2008/50/CE, are better reproduced and the uncertainty of the modelling system, as established by the European Directive 2008/50/CE, is reduced from 20% to 7.5%. Such uncertainty in the model results is under the established EU limit of the 50%. Significant improvements in the O(3) timing and amplitude of the daily cycle are also observed after the post-processing. The systematic improvements in the O(3) maximum simulations suggest that the Kalman filter post-processing method is a suitable technique to reproduce accurate estimate of ground-level O(3) concentration. With this study we evince that the adjusted O(3) concentrations obtained after the post-process of the results from the CALIOPE system are a reliable means for real near time O(3) forecasts.

Ozone attributed to Madrid and Barcelona on-road transport emissions: Characterization of plume dynamics over the Iberian Peninsula.

Despite the ~30% emission decrease of the main tropospheric ozone (O3) precursors in Spain in the 2001-2012 period, the O3 concentration in summer still exceeds the target value for the protection of the human health of the Air Quality Directive (2008/50/EC). On-road transport is the main anthropogenic contributor to O3 precursors emissions in Madrid and Barcelona metropolitan areas (65%/59% of NOx, 40%/33% of NMVOC, and 67%/85% of CO emissions) but this contribution to O3 formation is not well understood. The present work aims at increasing the understanding on the role of on-road transport emissions from main Spanish urban areas in O3 dynamics over Spain under typical circulation types. For that purpose, the Integrated Source Apportionment Method is used within the CALIOPE modelling system (WRF/CMAQ/HERMES/BSC-DREAM8b). The results indicate that the daily maximum O3 concentration attributed to the on-road transport emissions from Madrid (O3T-MAD) and Barcelona metropolitan areas (O3T-BCN) contribute up to 24% and 8% to total O3 concentration, respectively, within an area of influence of 200 km. The contribution of O3T-MAD and O3T-BCN is particularly significant (up to 80-100 μg m(-3) in an hour) to the O3 concentration peak during the central hours of the day in the high O3 concentration season (April-September). The maximum O3T-MAD concentration is calculated within the metropolitan area of Madrid but the plume, channelled by the Tajo and the Henares valleys, affects large areas of the Iberian Peninsula. The O3T-BCN plume is more driven by sea-land and mountain-valley breezes than by the synoptic advection and its maximum concentration is usually registered over the Mediterranean Sea. The O3 concentration transported long-range to the Iberian Peninsula is significant in the area of influence of Madrid and Barcelona, being maxima under cold (70-96%) and minima in warm circulation types (35-70%).

Ozone source apportionment during peak summer events oversouthwestern Europe

It is well established that in Europe, high O3 concentrations are most pronounced in southern/Mediterranean countries due to the more favorable climatological conditions for its formation. However, the contribution of the different sources of precursors to O3 formation within each country relative to the imported (regional and hemispheric) O3 is poorly quantified. This lack of quantitative knowledge prevents local authorities from effectively designing plans that reduce the 15 exceedances of the O3 Target Value set by the European Air Quality Directive. O3 source attribution is a challenge because the concentration at each location and time results not only from local biogenic and anthropogenic precursors, but also from the transport of O3 and precursors from neighbouring regions, O3 regional and hemispheric transport and stratospheric O3 injections. The main goal of this study is to provide a first quantitative estimation of the contribution of the main anthropogenic activity sectors to peak O3 events in Spain relative to the contribution of imported (regional and hemispheric) O3. We also 20 assess the potential of our source apportionment method to improve O3 modelling. Our study applies and thoroughly evaluates a countrywide O3 source apportionment method implemented in the CALIOPE air quality forecast system for Spain at high resolution (4 x 4 km) over a 10-day period characterized by typical summer conditions in the Iberian Peninsula (IP). The method tags both O3 and its gas precursor emissions from source sectors within one simulation and each tagged species is subject to the typical physical processes (advection, vertical mixing, deposition, emission and chemistry) as the actual 25 conditions remain unperturbed. We quantify the individual contributions of the largest NOx local sources to high O3 concentrations compared to the contribution of imported O3. We show for the first time that imported O3 is the largest input to the ground-level O3 concentration in the IP, accounting for 46% to 68 % of the daily mean O3 concentration during exceedances of the European Target Value. The hourly imported O3 increases during typical northwestern advections (70-90%, 60-80 μg/m), and decreases during typical stagnant conditions (30-40%, 30-60 μg/m) due to the local NO titration. During stagnant 30 conditions, the local anthropogenic precursors control the O3 peaks in areas downwind of the main urban and industrial regions (up to 40% in hourly peaks). We also show that ground-level O3 concentrations are strongly affected by vertical mixing of O3rich layers present in the free troposphere, which result from local/regional layering and accumulation, and