Fossil and Non-fossil Fuel Sources of Organic and Elemental Carbonaceous Aerosol in Beijing, Shanghai, and Guangzhou: Seasonal Carbon Source Variation

We measured the radiocarbon isotope signals in various fractions of carbonaceous aerosols sampled across four seasons (Oct 2013–Jul 2014) in three megacities of China, viz., Beijing, Shanghai, and Guangzhou. The contributions of fossil fuel (FF) and non-fossil fuel (NF) to the carbonaceous aerosol were estimated based on the radiocarbon content in the organic carbon (OC), water-soluble organic carbon (WSOC), water-insoluble organic carbon (WIOC), and elemental carbon (EC). Although NF generated the primary share (> 55%) during autumn in all of the cities, the seasonal contributions of the sources differed by location during the rest of the year. During winter, FF emissions constituted the majority of the carbonaceous pollution (64%) in Beijing, probably as a result of increased coal combustion for heating. On average, the EC, WSOC, and WIOC generated by FF composed ~10%, 35%, and 19% of the total carbon (TC). Overall, NF was identified as the largest source of carbonaceous aerosol in Guangzhou (63%), whereas FF was the largest source, contributing slightly more than NF, in Shanghai (54%). During spring and summer, FF played a greater role than NF in Beijing (~55%) and Guangzhou (~63%); additionally, based on our limited number of samples, it contributed 71% in Shanghai during the latter season, with a significant portion due to fuel combustion (i.e., industrial, vehicular, fishing-boat, and large-vessel emissions)