Source apportionment of fine particulate matter organic carbon in Shenzhen, China by chemical mass balance and radiocarbon methods

Abstract

Chemical mass balance (CMB) modeling and radiocarbon measurements were combined to evaluate the sources of carbonaceous fine particulate matter (PM2.5) in Shenzhen, China during and after the 2011 summer Universiade games when air pollution control measurements were implemented to achieve air quality targets. Ambient PM2.5 filter samples were collected daily at two sampling sites (Peking University Shenzhen campus and Longgang) over 24 consecutive days, covering the controlled and uncontrolled periods. During the controlled period, the average PM2.5 concentration was less than half of what it was after the controls were lifted. Organic carbon (OC), organic molecular markers (e.g., levoglucosan, hopanes, polycyclic aromatic hydrocarbons), and secondary organic carbon (SOC) tracers were all significantly lower during the controlled period. After pollution controls ended, at Peking University, OC source contributions included gasoline and diesel engines (24%), coal combustion (6%), biomass burning (12.2%), vegetative detritus (2%), biogenic SOC (from isoprene, α-pinene, and β-caryophyllene; 7.1%), aromatic SOC (23%), and other sources not included in the model (25%). At Longgang after the controls ended, similar source contributions were observed: gasoline and diesel engines (23%), coal combustion (7%), biomass burning (17.7%), vegetative detritus (1%), biogenic SOC (from isoprene, α-pinene, and β-caryophyllene; 5.3%), aromatic SOC (13%), and other sources (33%). The contributions of the following sources were smaller during the pollution controls: biogenic SOC (by a factor of 10-16), aromatic SOC (4-12), coal combustion (1.5-6.8), and biomass burning (2.3-4.9). CMB model results and radiocarbon measurements both indicated that fossil carbon dominated over modern carbon, regardless of pollution controls. However, the CMB model needs further improvement to apportion contemporary carbon (i.e. biomass burning, biogenic SOC) in this region. This work defines the major contributors to carbonaceous PM2.5 in Shenzhen and demonstrates that control measures for primary emissions could significantly reduce secondary organic aerosol (SOA) formation. Air quality regulations during Universiade 2011 in Shenzhen, China corresponded to significant decreases in fine particle organic carbon from coal combustion, biomass burning, and secondary organic aerosol.