Comparison of five methodologies to apportion organic aerosol sources during a PM pollution event.

This study presents a comparison of five methodologies to apportion primary (POA) and secondary organic aerosol (SOA) sources from measurements performed in the Paris region (France) during a highly processed PM pollution event. POA fractions, estimated from EC-tracer method and positive matrix factorization (PMF) analyses, conducted on measurements from PM10 filters, aerosol chemical speciation monitor (ACSM) and offline aerosol mass spectrometry (AMS), were all comparable (2.2-3.7 µg m-3 as primary organic carbon (POC)). Associated relative uncertainties (measurement + model) on POC estimations ranged from 8 to 50%. The best apportionment of primary traffic OA was achieved using key markers (EC and 1-nitropyrene) in the chemical speciation-based PMF showing more pronounced rush-hour peaks and greater correlation with NOx than other traffic related POC factors. All biomass burning-related factors were in good agreement, with a typical diel profile and a night-time increase linked to residential heating. If PMF applied to ACSM data showed good agreement with other PMF outputs corrected from dust-related factors (coarse PM), discrepancies were observed between individual POA factors (traffic, biomass burning) and directly comparable SOA factors and highly oxidized OA. Similar secondary organic carbon (SOC) concentrations (3.3 ± 0.1 µg m-3) were obtained from all approaches, except the SOA-tracer method (1.8 µg m-3). Associated uncertainties ranged from 14 to 52% with larger uncertainties obtained for PMF-chemical data, EC- and SOA-tracer methods. This latter significantly underestimated total SOA loadings, even including biomass burning SOA, due to missing SOA classes and precursors. None of the approaches was able to identify the formation mechanisms and/or precursors responsible for the highly oxidized SOA fraction associated with nitrate- and/or sulfate-rich aerosols (35% of OA). We recommend the use of a combination of different methodologies to apportion the POC/SOC concentrations/contributions to get the highest level of confidence in the estimates obtained.

Gasoline cars produce more carbonaceous particulate matter than modern filter-equipped diesel cars.

Carbonaceous particulate matter (PM), comprising black carbon (BC), primary organic aerosol (POA) and secondary organic aerosol (SOA, from atmospheric aging of precursors), is a highly toxic vehicle exhaust component. Therefore, understanding vehicle pollution requires knowledge of both primary emissions, and how these emissions age in the atmosphere. We provide a systematic examination of carbonaceous PM emissions and parameterisation of SOA formation from modern diesel and gasoline cars at different temperatures (22, -7 °C) during controlled laboratory experiments. Carbonaceous PM emission and SOA formation is markedly higher from gasoline than diesel particle filter (DPF) and catalyst-equipped diesel cars, more so at -7 °C, contrasting with nitrogen oxides (NOX). Higher SOA formation from gasoline cars and primary emission reductions for diesels implies gasoline cars will increasingly dominate vehicular total carbonaceous PM, though older non-DPF-equipped diesels will continue to dominate the primary fraction for some time. Supported by state-of-the-art source apportionment of ambient fossil fuel derived PM, our results show that whether gasoline or diesel cars are more polluting depends on the pollutant in question, i.e. that diesel cars are not necessarily worse polluters than gasoline cars.