[1] Aqueous-phase oxidation (in clouds and aerosols) is a potentially important source of organic aerosol and could explain the atmospheric presence of oxalic acid. Methylglyoxal, a water-soluble product of isoprene, oxidizes further in the aqueous phase to pyruvic acid. Discrepancies in the literature regarding the aqueous-phase oxidation of pyruvic acid create large uncertainties in the incloud yields of secondary organic aerosol (SOA) and oxalic acid. Resolving the fate of aqueous-phase pyruvic acid is critical to understanding SOA formation through cloud processing of water-soluble products of isoprene, other alkenes and aromatics. In this work, aqueous-phase photochemical reactions of pyruvic acid and hydrogen peroxide at pH values typical of clouds were conducted and demonstrated that photochemical oxidation of pyruvic acid yields glyoxylic, oxalic, acetic and formic acids. Oxalic and glyoxylic acids remain mostly in the particle phase upon droplet evaporation. Thus isoprene is an important precursor of in-cloud SOA formation. Citation:
The organic compound tracers of atmospheric particulate matter, as well as organic carbon (OC) and elemental carbon (EC), have been characterized for samples acquired during the ACEAsia campaign from Gosan, Jeju Island, Korea; Sapporo, Japan, and Chichi-jima Island in the western North Pacific, as well as on the NOAA R/V Ronald H. Brown. Total extracts were analyzed by GC-MS to determine both polar and aliphatic compounds. Total particles, organic matter and lipid and saccharide compounds were high during the Asian dust episode (early April 2001) compared to levels at other times. The organic matter can be apportioned to seven emission sources and to significant oxidation producing secondary products during long-range transport. Terrestrial natural background compounds are vascular plant wax lipids derived from direct emission and as part of desert sand dust. Fossil fuel utilization is obvious and derives from petroleum product and coal combustion emissions. Saccharides are a major polar (water-soluble) carbonaceous fraction derived from soil resuspension (agricultural activities). Biomass burning smoke is evident in all samples and seasons. It contributes up to 13% of the total compound mass as water-soluble constituents. Burning of refuse is another source of organic particles. Varying levels of marine-derived lipids are superimposed during aerosol transport over the ocean.Secondary oxidation products increase with increasing transport distance and time. The ACEAsia aerosols are comprised not only of desert dust, but also of soil dust, smoke from biomass and refuse burning, and emissions from fossil fuels use in urban areas.
A laboratory intercomparison of organic carbon (OC) and elemental carbon (EC) measurements of atmospheric particulate matter samples collected on quartz filters was conducted among eight participants of the ACE-Asia field experiment The intercomparison took place in two stages: the first round of the intercomparison was conducted when filter samples collected during the ACE-Asia experiment were being analyzed for OC and EC, and the second round was conducted after the ACE-Asia experiment and included selected samples from the ACE-Asia experiment Each participant operated ECOC analyzers from the same manufacturer and utilized the same analysis protocol for their measurements. The precision of OC measurements of quartz fiber filters was a function of the filter's carbon loading but was found to be in the range of 4-13% for OC loadings of 1.0-25 microg of C cm(-2). For measurements of EC, the precision was found to be in the range of 6-21% for EC loadings in the range of 0.7-8.4 microg of C cm(-2). It was demonstrated for three ambient samples, four source samples, and three complex mixtures of organic compounds that the relative amount of total evolved carbon allocated as OC and EC (i.e., the ECOC split) is sensitive to the temperature program used for analysis, and the magnitude of the sensitivity is dependent on the types of aerosol particles collected. The fraction of elemental carbon measured in wood smoke and an extract of organic compounds from a wood smoke sample were sensitive to the temperature program used for the ECOC analysis. The ECOC split for the three ambient samples and a coal fly ash sample showed moderate sensitivity to temperature program, while a carbon black sample and a sample of secondary organic aerosol were measured to have the same split of OC and EC with all temperature programs that were examined.
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