Airborne polycyclic aromatic hydrocarbons (PAHs) are of great concern to human health due to their potential high toxicity. Understanding the characteristics and sources of PAHs, as well as the governing factors, is therefore critical. PAHs and refractory black carbon (rBC) are both from combustion sources. This work, for the first time, investigated exclusively the rBC-bound PAH properties by using a laser-only Aerodyne soot-particle aerosol mass spectrometer (SP-AMS). This technique offers highly time-resolved PAH results that a traditional offline measurement is unable to provide. We analyzed two datasets conducted in urban Shanghai during the fall of 2018 and in suburban Nanjing during the winter of 2017, respectively. Results show that the average concentration of PAHs in Nanjing was much higher than that in Shanghai. Nanjing PAHs contained more low molecular weight components while Shanghai PAHs contained more high molecular weight ones. PAHs in Shanghai presented two peaks in early morning and evening, while Nanjing PAHs had only one significant morning peak, but remained high throughout the nighttime. A multi-linear regression algorithm combined with positive matrix factorization (PMF) analyses on sources of PAHs reveals that the industry emissions contributed the majority of PAHs in Nanjing (~80%), while traffic emissions dominated PAHs in Shanghai (~70%). We further investigated the relationships between PAHs with various factors. PAHs in both sites tended to positively correlate with primary pollutants, including primary organic aerosol (OA) factors, and gaseous pollutants of CO, NO2 and SO2, but negatively correlated with secondary OA factors and O3. This result highlights the enhancement of rBC-bound PAHs level due to primary emissions and their oxidation loss upon atmospheric aging reactions. High concentration of PAHs seemed to frequently appear under low temperature and high relative humidity conditions, especially in Shanghai.
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