Does Ambient Secondary Conversion or the Prolonged Fast Conversion in Combustion Plumes Cause Severe PM2.5 Air Pollution in China?

The ambient formation of secondary particulate matter (ambient FSPM) is commonly recognized as the major cause of severe PM2.5 air pollution in China. We present observational evidence showing that the ambient FSPM was too weak to yield a detectable contribution to extreme PM2.5 pollution events that swept northern China between 11 and 14 January 2019. Although the Community Multiscale Air Quality (CMAQ) model (v5.2) reasonably reproduced the observations in January 2019, it largely underestimated the concentrations of the PM2.5 during the episode. We propose a novel mechanism, called the in-fresh-stack-plume non-precipitation-cloud processing of aerosols followed by the evaporation of semi-volatile components from the aerosols, to generate PM2.5 at extremely high concentrations because of highly concentrated gaseous precursors and large amounts of water droplets in fresh cooling combustion plumes under poor dispersion conditions, low ambient temperature, and high relative humidity. The recorded non-precipitation-cloud processing of the aerosols in fresh stack combustion plumes normally lasts 20-30 s, but it prolongs as long as 2-5 min under cold, humid, and stagnant meteorological conditions and expectedly causes severe PM2.5 pollution events. Regardless of the presence of the natural cloud in the planetary boundary layer during the extreme events, the fast conversion of air pollutants in water droplets and the generation of the PM2.5 through the non-precipitation-cloud processing of aerosols always occur in fresh combustion plumes. The processing of aerosols is detectable using a nano-scan particle sizer assembled on an unmanned aerial vehicle to monitor the particle formation in stack plumes. In-fresh-stack-plume processed aerosols under varying meteorological conditions need to be studied urgently.

Automated summary

The ambient formation of secondary particulate matter is considered to be the main cause of severe PM2.5 air pollution in China. However, observational evidence shows that in the extreme PM2.5 pollution events that occurred in northern China between January 11 and 14, 2019, the ambient formation of secondary particulate matter did not make a significant contribution. Therefore, a new mechanism needs to be studied to understand the formation process of PM2.5.