Simulation of the chemical evolution of biomass burning organic aerosol

摘要

The chemical transport model PMCAMx was extended to investigate the effects of partitioning and photochemical aging of biomass burning emissions on organic aerosol (OA) concentrations. A source-resolved version of the model, PMCAMx-SR, was developed in which biomass burning emissions and their oxidation products are represented separately from the other OA components. The volatility distribution and chemical aging of biomass burning OA (BBOA) were simulated based on recent laboratory measurements. PMCAMx-SR was applied to Europe during an early summer period (1–29?May 2008) and a winter period (25?February–22?March 2009). During the early summer, the contribution of biomass burning (both primary and secondary species) to total OA levels over continental Europe was estimated to be approximately 16?%. During winter the contribution was nearly 47?%, due to both extensive residential wood combustion but also wildfires in Portugal and Spain. The intermediate volatility compounds (IVOCs) with effective saturation concentration values of 10 sup5/sup and 10 sup6/sup μ g?m sup?3/sup are predicted to contribute around one third of the BBOA during the summer and 15?% during the winter by forming secondary OA (SOA). The uncertain emissions of these compounds and their SOA formation potential require additional attention. Evaluation of PMCAMx-SR predictions against aerosol mass spectrometer measurements in several sites around Europe suggests reasonably good performance for OA (fractional bias less than 35?% and fractional error less than 50?%). The performance was weaker during the winter suggesting uncertainties in residential heating emissions and the simulation of the resulting BBOA in this season.