ABSTRACT
Countries in Northeast Asia have been regulating PM2.5 sources and studying their local and transboundary origins since PM2.5 causes severe impacts on public health and economic losses. However, the separation of local and transboundary impacts is not fully realized because it is impossible to change air pollutant emissions from multiple countries experimentally. Exceptionally, the early stage of the COVID-19 outbreak (January-March 2020) provided a cross-country experiment to separate each impact of PM2.5 sources identified in Seoul, a downwind area of China. We evaluated the contributions of PM2.5 sources compared to 2019 using dispersion normalized positive matrix factorization (DN-PMF) during three meteorological episodes. Episodes 1 and 2 revealed transboundary impacts and were related to reduced anthropogenic emissions and accumulated primary pollutants in Northeast China. Anthropogenic emissions, except for the residential sector, decreased, but primary air pollutants accumulated by residential coal combustion enhanced secondary aerosol formation. Thus, the contributions of sulfate and secondary nitrate increased in Seoul during episode 1 but then decreased maximally with other primary sources (biomass burning, district heating and incineration, industrial sources, and oil combustion) during episode 2 under meteorological conditions favorable to long-range transport. Local impact was demonstrated by atmospheric stagnation during episode 3. Meteorological condition unfavorable to local dispersion elevated the contributions of mobile and coal combustion and further contributed to PM2.5 high concentration events (HCE). Our study separates the local and transboundary impacts and highlights that cooperations in Northeast Asia on secondary aerosol formation and management of local sources are necessary.
ABSTRACT
We investigated the changes in the size distribution, coating thickness, and mass absorption cross-section (MAC) of black carbon (BC) with aging and estimated the light absorption enhancement (Eabs) in the Asian outflow from airborne in-situ measurements during 2016 KORUS-AQ campaign. The BC number concentration decreased, but mass mean diameter increased with increasing altitude in the West Coast (WC) and Seoul Metropolitan Area (SMA), reflecting the contrast between freshly emitted BC-containing particles at the surface and more aged aerosol associated with aggregation during vertical mixing and transport. Contradistinctively, BC number and mass size distributions were relatively invariant with altitude over the Yellow Sea (YS) because sufficiently aged BC from eastern China were horizontally transported to all altitudes over the YS, and there are no significant sources at the surface. The averaged inferred MAC of refractory BC in three regions reflecting differences in their size distributions increased to 9.8 ± 1.0 m2 g-1 (YS), 9.3 ± 0.9 m2 g-1 (WC), and 8.2 ± 0.9 m2 g-1 (SMA) as BC coating thickness increased from 20 nm to 120 nm. The absorption coefficient of BC calculated from the coating thickness and MAC were highly correlated with the filter-based absorption measurements with the slope of 1.16 and R2 of 0.96 at 550 nm, revealing that the thickly coated BC had a large MAC and absorption coefficient. The Eabs due to the inferred coatings was estimated as 1.0-1.6, which was about 30% lower than those from climate models and laboratory experiments, suggesting that the increase in the BC absorption by the coatings in the Asian outflow is not as large as calculated in the previous studies. Organics contributed to the largest Eabs accounting for 69% (YS), 61% (WC), and 64% (SMA). This implies that organics are largely responsible for the lensing effect of BC rather than sulfates in the Asian outflow.
