Measurement of the ambient organic aerosol volatility distribution: application during the Finokalia Aerosol Measurement Experiment (FAME-2008)

A variable residence time thermodenuder (TD) was combined with an Aerodyne Aerosol Mass Spectrometer (AMS) and a Scanning Mobility Particle Sizer (SMPS) to measure the volatility distribution of aged organic aerosol in the Eastern Mediterranean during the Finokalia Aerosol Measurement Experiment in May of 2008 (FAME-2008). A new method for the quantification of the organic aerosol volatility distribution was developed combining measurements of all three instruments together with an aerosol dynamics model. Challenges in the interpretation of ambient thermodenuder-AMS measurements include the potential resistances to mass transfer during particle evaporation, the effects of particle size on the evaporated mass fraction, the changes in the AMS collection efficiency and particle density as the particles evaporate partially in the TD, and finally potential losses inside the TD. Our proposed measurement and data analysis method accounts for all of these problems combining the AMS and SMPS measurements. The AMS collection efficiency of the aerosol that passed through the TD was found to be approximately 10% lower than the collection efficiency of the aerosol that passed through the bypass. The organic aerosol measured at Finokalia is approximately 2 or more orders of magnitude less volatile than fresh laboratory-generated monoterpene (α-pinene, β-pinene and limonene under low NOx conditions) secondary organic aerosol. This low volatility is consistent with its highly oxygenated AMS mass spectrum. The results are found to be highly sensitive to the mass accommodation coefficient of the evaporating species. This analysis is based on the assumption that there were no significant reactions taking place inside the thermodenuder.</p

Aged organic aerosol in the Eastern Mediterranean: the Finokalia Aerosol Measurement Experiment – 2008

Aged organic aerosol (OA) was measured at a remote coastal site on the island of Crete, Greece during the Finokalia Aerosol Measurement Experiment-2008 (FAME-2008), which was part of the EUCAARI intensive campaign of May 2008. The site at Finokalia is influenced by air masses from different source regions, including long-range transport of pollution from continental Europe. A quadrupole aerosol mass spectrometer (Q-AMS) was employed to measure the size-resolved chemical composition of non-refractory submicron aerosol (NR-PM1), and to estimate the extent of oxidation of the organic aerosol. Factor analysis was used to gain insights into the processes and sources affecting the OA composition. The particles were internally mixed and liquid. The largest fraction of the dry NR-PM1 sampled was ammonium sulfate and ammonium bisulfate, followed by organics and a small amount of nitrate. The variability in OA composition could be explained with two factors of oxygenated organic aerosol (OOA) with differing extents of oxidation but similar volatility. Hydrocarbon-like organic aerosol (HOA) was not detected. There was no statistically significant diurnal variation in the bulk composition of NR-PM1 such as total sulfate or total organic aerosol concentrations. However, the OA composition exhibited statistically significant diurnal variation with more oxidized OA in the afternoon. The organic aerosol was highly oxidized, regardless of the source region. Total OA concentrations also varied little with source region, suggesting that local sources had only a small effect on OA concentrations measured at Finokalia. The aerosol was transported for about one day before arriving at the site, corresponding to an OH exposure of approximately 4×1011 molecules cm−3 s. The constant extent of oxidation suggests that atmospheric aging results in a highly oxidized OA at these OH exposures, regardless of the aerosol source.</p

Time-Resolved Characterization of Primary Emissions from Residential Wood Combustion Appliances

Primary emissions from a log wood burner and a pellet boiler were characterized by online measurements of the organic aerosol (OA) using a high-resolution time-of-flight aerosol mass spectrometer (HR-TOF-AMS) and of black carbon (BC). The OA and BC concentrations measured during the burning cycle of the log wood burner, batch wise fueled with wood logs, were highly variable and generally dominated by BC. The emissions of the pellet burner had, besides inorganic material, a high fraction of OA and a minor contribution of BC. However, during artificially induced poor burning BC was the dominating species with ∼80% of the measured mass. The elemental O:C ratio of the OA was generally found in the range of 0.2–0.5 during the startup phase or after reloading of the log wood burner. During the burnout or smoldering phase, O:C ratios increased up to 1.6–1.7, which is similar to the ratios found for the pellet boiler during stable burning conditions and higher than the O:C ratios observed for highly aged ambient OA. The organic emissions of both burners have a very similar H:C ratio at a given O:C ratio and therefore fall on the same line in the Van Krevelen diagram

Time-Resolved Characterization of Primary Emissions from Residential Wood Combustion Appliances

Primary emissions from a log wood burner and a pellet boiler were characterized by online measurements of the organic aerosol (OA) using a high-resolution time-of-flight aerosol mass spectrometer (HR-TOF-AMS) and of black carbon (BC). The OA and BC concentrations measured during the burning cycle of the log wood burner, batch wise fueled with wood logs, were highly variable and generally dominated by BC. The emissions of the pellet burner had, besides inorganic material, a high fraction of OA and a minor contribution of BC. However, during artificially induced poor burning BC was the dominating species with ∼80% of the measured mass. The elemental O:C ratio of the OA was generally found in the range of 0.2–0.5 during the startup phase or after reloading of the log wood burner. During the burnout or smoldering phase, O:C ratios increased up to 1.6–1.7, which is similar to the ratios found for the pellet boiler during stable burning conditions and higher than the O:C ratios observed for highly aged ambient OA. The organic emissions of both burners have a very similar H:C ratio at a given O:C ratio and therefore fall on the same line in the Van Krevelen diagram