Reactive organic carbon air emissions from mobile sources in the United States.

ABSTRACT

Mobile sources are responsible for a substantial controllable portion of the reactive organic carbon (ROC) emitted to the atmosphere, especially in urban environments of the United States. We update existing methods for calculating mobile source organic particle and vapor emissions in the United States with over a decade of laboratory data that parameterize the volatility and organic aerosol (OA) potential of emissions from on-road vehicles, nonroad engines, aircraft, marine vessels, and locomotives. We find that existing emission factor information from Teflon filters combined with quartz filters collapses into simple relationships and can be used to reconstruct the complete volatility distribution of ROC emissions. This new approach consists of source-specific filter artifact corrections and state-of-the-science speciation including explicit intermediate-volatility organic compounds (IVOCs), yielding the first bottom-up volatility-resolved inventory of US mobile source emissions. Using the Community Multiscale Air Quality model, we estimate mobile sources account for 20 %-25 % of the IVOC concentrations and 4.4 %-21.4 % of ambient OA. The updated emissions and air quality model reduce biases in predicting fine-particle organic carbon in winter, spring, and autumn throughout the United States (4.3 %-11.3 % reduction in normalized bias). We identify key uncertain parameters that align with current state-of-the-art research measurement challenges.