Primary versus secondary and anthropogenic versus natural sources of aminium ions in atmospheric particles during nine coastal and marine campaigns

In this study, size-segregated dimethylaminium (DMA+) and trimethylaminium (TMA+) in atmospheric particles were measured during four coastal campaigns in Qingdao, China and five campaigns cruising over marginal seas of China and the northwest Pacific Ocean. The measured averages of DMA+ and TMA+ in PM0.056-10 (the sum of chemical concentrations from 0.056 to 10 µm) during each campaign, ranged from 0.045 to 1.1 nmol m-3 and from 0.029 to 0.53 nmol m-3, respectively. Size distributions of DMA+ and TMA+ in coastal atmospheric particles suggested that primary combustion emissions featured by mass median aerodynamic diameter (MMAD) at 0.2 µm generally yielded appreciable contributions to their observed concentrations in PM0.056-10 and sometimes dominantly contributed. In the marine atmospheres, the 0.1-0.2 µm modes of DMA+ and TMA+ also existed and sometimes dominated while they were very likely derived from primary ocean-biogenic emissions. In most of the samples during nine campaigns, secondarily-formed DMA+ and TMA+ in droplet mode with MMAD at 0.3-2 µm dominantly contributed to DMA+ and TMA+ in PM0.056-10. Overall, our results suggested that DMA+ and TMA+ in the marine atmospheric particles overwhelmingly came from ocean biogenic sources while they were likely derived from complicated anthropogenic and natural sources at the coastal sites.