Characteristics and unique sources of polycyclic aromatic hydrocarbons and nitro-polycyclic aromatic hydrocarbons in PM2.5 at a highland background site in northwestern China☆

Highlights: • PAHs and NPAHs were first observed at SACOL in the northwestern highlands of China. • The ratio of Pyr to FR was unusually high in spring and fall sampling campaigns. • The high Pyr to FR ratio may be due to the burning of Tibetan barley straw. • Air pollution with Tibetan features produced an impact on the surrounding areas. Polycyclic aromatic hydrocarbons (PAHs) and nitro-PAHs (NPAHs) in PM_2.5 were first observed at a background site (Yuzhong site: YZ site) in the northwestern highlands of China in five seasonal campaigns. Compared with major northwestern cities, PAHs and NPAHs at the YZ site were at a lower level but showed consistent seasonal differences. The PAH and NPAH concentrations peaked in the winter campaigns, which were 36.11 ± 6.54 ng/m³ and 418.11 ± 123.55 pg/m³, respectively, in winter campaign 1 and 28.97 ± 10.07 ng/m³ and 226.89 ± 133.54 pg/m³, respectively, in winter campaign 2. These values were approximately a dozen times larger those in other campaigns. The diagnostic ratios indicate that vehicle emissions were the primary source of the PAHs throughout the five campaigns, and coal and biomass combustion also contributed during the winter, summer, and fall campaigns. Among NPAHs, 2-nitrofluoranthene and 2-nitropyrene were generated through OH radical-initiated reactions during atmospheric transport, while 1-nitropyrene came from combustion sources. There is an observation worth pondering, which is that the ratio between pyrene and fluoranthene increased abnormally in the spring and fall campaigns, which is presumably caused by the burning of Tibetan barley straw in the northwestern highlands. The backward trajectories over Tibetan areas in Qinghai and southwestern Gansu are consistent with this hypothesis. In addition, this study reported for the first time that the burning of Tibetan barley straw has become a seasonal contributor to air pollution in northwestern China and is participating in the atmospheric transport of air pollutants driven by the monsoon in East Asia, which urgently requires further research.