Quantifying traffic, biomass burning and secondary source contributions to atmospheric particle number concentrations at urban and suburban sites.

In this study, we propose a new approach to determine the contributions of primary vehicle exhaust (N1ff), primary biomass burning (N1bb) and secondary (N2) particles to mode segregated particle number concentrations. We used simultaneous measurements of aerosol size distribution in the 12-600 nm size range and black carbon (BC) concentration obtained during winter period at urban and suburban sites influenced by biomass burning (BB) emissions. As expected, larger aerosol number concentrations in the 12-25 and 25-100 nm size ranges are observed at the urban site compared to the suburban site. However, similar concentrations of BC are observed at both sites due to the larger contribution of BB particles to the observed BC at suburban (34%) in comparison to urban site (23%). Due to this influence of BB emissions in our study area, the application of the Rodríguez and Cuevas (2007) method, which was developed for areas mainly influenced by traffic emissions, leads to an overestimation of the primary vehicle exhaust particles concentrations by 18% and 26% in urban and suburban sites, respectively, as compared to our new proposed approach. The results show that (1) N2 is the main contributor in all size ranges at both sites, (2) N1ff is the main contributor to primary particles (>70%) in all size ranges at both sites and (3) N1bb contributes significantly to the primary particles in the 25-100 and 100-600 nm size ranges at the suburban (24% and 28%, respectively) and urban (13% and 20%, respectively) sites. At urban site, the N1ff contribution shows a slight increase with the increase of total particle concentration, reaching a contribution of up to 65% at high ambient aerosol concentrations. New particle formation events are an important aerosol source during summer noon hours but, on average, these events do not implicate a considerable contribution to urban particles.

Impact of primary NO2 emissions at different urban sites exceeding the European NO2 standard limit.

A large part of the European population is still exposed to ambient nitrogen dioxide (NO2) levels exceeding the European Union (EU) air quality standards, being a key challenge to reduce NO2 concentrations across many European urban areas, particularly close to roads. In this work, a trend analysis of pollutants involved in NO2 processes was done for the period 2003-2014 in traffic sites from three Spanish cities (Barcelona, Madrid and Granada) that still exceed the European NO2 air quality standard limits. We also estimated the contributions of primary NO2 emissions and photo-chemically formed NO2 to the observed ambient NO2 concentrations in order to explore their possible role in the observed NO2 concentration trends. The NOx and NO concentrations at these traffic sites showed significant decreasing trends during the period 2003-2014, especially at Barcelona (BARTR) and Madrid (MADTR) traffic stations. The NO2 concentrations showed statistically significant downward trends at BARTR and MADTR and remained unchanged at Granada traffic station (GRATR) during the study period. Despite the significant decrease in NO2 concentrations in BCNTR and MADTR during the analysed period, the NO2 concentrations observed over these sites still above the annual NO2 standard limit of 40 µg m-3 and, therefore, more efficient measures are still needed. Primary NO2 emissions significantly influence NO2 concentrations at the three analysed sites. However, as no drastic changes are expected in the after-exhaust treatment technology that can reduce primary NO2 emissions to zero in the near future, only a substantial reduction in NOx emissions will help to comply with the NO2 European air quality standards. Reduction of 78%, 56% and 16% on NOx emissions in Barcelona, Madrid and Granada were estimated to be necessary to comply with the NO2 annual limit of 40 µg m-3.

Spatial and temporal variability of carbonaceous aerosols: Assessing the impact of biomass burning in the urban environment.

Biomass burning (BB) is a significant source of atmospheric particles in many parts of the world. Whereas many studies have demonstrated the importance of BB emissions in central and northern Europe, especially in rural areas, its impact in urban air quality of southern European countries has been sparsely investigated. In this study, highly time resolved multi-wavelength absorption coefficients together with levoglucosan (BB tracer) mass concentrations were combined to apportion carbonaceous aerosol sources. The Aethalometer model takes advantage of the different spectral behavior of BB and fossil fuel (FF) combustion aerosols. The model was found to be more sensitive to the assumed value of the aerosol Ångström exponent (AAE) for FF (AAEff) than to the AAE for BB (AAEbb). As result of various sensitivity tests the model was optimized with AAEff=1.1 and AAEbb=2. The Aethalometer model and levoglucosan tracer estimates were in good agreement. The Aethalometer model was further applied to data from three sites in Granada urban area to evaluate the spatial variation of CMff and CMbb (carbonaceous matter from FF or BB origin, respectively) concentrations within the city. The results showed that CMbb was lower in the city centre while it has an unexpected profound impact on the CM levels measured in the suburbs (about 40%). Analysis of BB tracers with respect to wind speed suggested that BB was dominated by sources outside the city, to the west in a rural area. Distinguishing whether it corresponds to agricultural waste burning or with biomass burning for domestic heating was not possible. This study also shows that although traffic restrictions measures contribute to reduce carbonaceous concentrations, the extent of the reduction is very local. Other sources such as BB, which can contribute to CM as much as traffic emissions, should be targeted to reduce air pollution.