Abstract
Abstract. Carbonyl compounds are important intermediates in atmospheric photochemistry. To explore the relative contributions of primary and secondary carbonyl sources, carbonyls and other volatile organic compounds (VOCs) were measured at an urban site in both winter and summer in Beijing. The positive matrix factorization (PMF) model was used for source apportionment of VOCs. As VOCs undergo photochemical processes in the atmosphere, and such processes may interfere with factor identification, the relationships between the contributions of the resolved PMF factors to each non-methane hydrocarbon (NMHC) species and its kOH value were used to distinguish fresh factors and photochemically aged factors. As the result of PMF, five factors were resolved in winter, and two of them were identified as photochemically aged emissions. In summer, four factors were resolved, including one aged factor. Carbonyls abundances from aged factors were simulated by VOCs consumption and the corresponding carbonyl production yields, and the simulated abundances agreed well with the results obtained by the PMF model. The source apportionment results indicated that secondary formation was the major source of carbonyls in both winter and summer, with the respective contributions of 51.2% and 46.0%. For the three major carbonyl species, primary anthropogenic sources contributed 28.9% and 32.3% to ambient formaldehyde, 53.7% and 41.6% to acetaldehyde, 68.1% and 56.2% to acetone in winter and summer, respectively.
Highlights
Carbonyls, including aldehydes and ketones, are a group of important oxygenated volatile organic compounds (OVOCs)
In contrast with the decreasing trend of carbonyl levels derived from ground-based measurements, satellite measurements suggested that formaldehyde columns showed an increasing trend (De Smedt et al, 2010)
To better understand the relationships between aged and fresh factors and the role of photochemical aging in Positive matrix factorization (PMF) analysis, we explored the relationships between VOC consumption and carbonyl formation in the aged factors
Summary
Carbonyls, including aldehydes and ketones, are a group of important oxygenated volatile organic compounds (OVOCs). As the key intermediates in the photo-oxidation of hydrocarbons, carbonyls are major sources of free radicals and are precursors of ozone, peroxyacyl nitrates and secondary organic aerosol (Singh et al, 1995; Finlayson-Pitts and Pitts, 1997; Liggio et al, 2005). Being produced from photo-oxidation of hydrocarbons, carbonyls can be directly emitted into the atmosphere from a variety of natural and anthropogenic sources. The major anthropogenic emission sources of carbonyls include incomplete combustion of fuels, industrial processes, and solvent usage (Zhang and Smith, 1999; Ban-Weiss et al, 2008; Kim et al, 2008). Due to the complexity of carbonyl sources and sinks, it is a challenge to quantifying the relative contributions of primary emissions and secondary formation
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