Seasonal variability in anthropogenic halocarbon emissions.

ABSTRACT

Ambient concentrations of eight predominantly anthropogenic halocarbons were measured via in situ gas chromatography in California's South Coast air basin for both summer and fall during the 2005 Study of Organic Aerosols at Riverside (SOAR). Ongoing emissions of the banned halocarbons methylchloroform and CFC-11 were observed in the South Coast air basin, whereas CFC-113 emissions have effectively ceased. We estimate anthropogenic emissions in the South Coast air basin for methylchloroform, CFC-11, HCFC-141b, chloroform, tetrachloroethene (PCE), trichloroethylene (TCE), and dichloromethane based on regressions of halocarbon to carbon monoxide mixing ratios and carbon monoxide emission inventories. We estimate per capita methylchloroform and chloroform emissions in the South Coast air basin for the year 2005 to be 6.6 +/- 0.4 g/(person.year) and 19 +/- 1 g/(person.year), respectively. We compare our results to national emission estimates calculated from previous work; for several compounds, emissions in the South Coast air basin are significantly lower than national per capita emissions. We observed strong seasonal differences in anthropogenic emissions of methylchloroform and chloroform; emissions were 4.5 and 2.5 times greater in summer than in fall, respectively. Possible seasonal sources include landfills and water chlorination. We conclude that seasonal variability in methylchloroform emissions has not been included in previous inventories and may cause errors in methylchloroform emission estimates after the year 2000 and seasonally resolved inversion calculations of hydroxyl radical abundance.