Abstract. Benzene and polycyclic aromatic hydrocarbons (PAHs) are toxic air pollutants that have long been associated with motor vehicle emissions, though the importance of such emissions has never been quantified over an extended domain using a chemical transport model. Herein we present the first application of such a model (GEM-MACH-PAH) to examine the contribution of motor vehicles to benzene and PAHs in ambient air. We have applied the model over a region that is centered on Toronto, Canada, and includes much of southern Ontario and the northeastern United States. The resolution (2.5 km) was the highest ever employed by a model for these compounds in North America, and the model domain was the largest at this resolution in the world to date. Using paired model simulations that were run with vehicle emissions turned on and off (while all other emissions were left on), we estimated the absolute and relative contributions of motor vehicles to ambient pollutant concentrations. Our results provide estimates of motor vehicle contributions that are realistic as a result of the inclusion of atmospheric processing, whereas assessing changes in benzene and PAH emissions alone would neglect effects caused by shifts in atmospheric oxidation and particle/gas partitioning. A secondary benefit of our scenario approach is in its utility in representing a fleet of zero emission vehicles (ZEV), whose adoption is being encouraged in a variety of jurisdictions. Our simulations predicted domain-average on-road vehicle contributions to benzene and PAH concentrations of 4–21 % and 14–24 % in the spring–summer and fall–winter periods, respectively, depending on the aromatic compound. Contributions to PAH concentrations up to 50 % were predicted for the Greater Toronto Area, with a domain maximum of 91 %. Such contributions are substantially higher than those reported in national emissions inventories, and they also differ from inventory estimates at the sub-national scale because those do not account for the physico-chemical processing that alters pollutant concentrations in the atmosphere. The removal of on-road vehicle emissions generally led to decreases in benzene and PAH concentrations during both periods that were studied, though atmospheric processing (such as chemical reactions and changes to gas/particle partitioning) contributed to non-linear behaviour at some locations or times of year. Such results demonstrate the added value associated with regional air quality modelling relative to examinations of emissions inventories alone. We also found that removing on-road vehicle emissions reduced spring–summertime surface O3 volume mixing ratios and fall–wintertime PM10 concentrations each by ~ 10 % in the model domain, providing further air quality benefits. Toxic equivalents contributed by vehicle emissions of PAHs were found to be substantial (20–60 % depending on location), and this finding is particularly relevant to the study of public health in the urban areas of our model area where human population, ambient concentrations, and traffic volumes tend to be high.
Trends in on-road vehicle emissions and ambient air quality in Atlanta, Georgia, USA, from the late 1990s through 2009
