Strong upwards transport of HONO in daytime over urban area of Beijing, China.

Strong upwards transport of Nitrous acid (HONO) in daytime over urban area of Beijing was observed based on combined observations of HONO, NOx (NO and NO2), nitrate, and PM2.5 at two heights (90 m and 528 m) on the highest building of Beijing (528 m above ground). The mean HONO at the 528 m (0.26 ppb) was lower than that at the 90 m (0.54 ppb), and a clear difference in diurnal variation of HONO between the two heights was observed. HONO at the 90 m showed two peaks in the morning rush hour and mid-night, but decreased sharply in daytime (e.g., from 0.62 ppb at 08:00 to 0.34 at 14:00); while the decreasing trend of HONO in daytime significantly weakened at the 528 m (e.g., from 0.26 ppb at 08:00 to 0.27 at 14:00).With PBL development in the morning, HONO in low layer was upwards transported to the 528 m, which compensated partly HONO loss via photolysis and resulted in a relatively stable concentration at the 528 m in daytime. A positive relationship of the bulk Richardson number (Ri) in 0-500 m with the difference of HONO between the two heights during daytime (08:00-18:00) confirmed the above analyses. HONO budget analysis indicated that a strong unknown HONO source existed at the 528 m in daytime, which was negative correlated to the Ri. These results further confirmed that vertical transport of HONO from low layer was a potential HONO source at the 528 m. Moreover, the contribution of photolysis of particulate nitrate significantly increased at the 528 m. Its contribution in total HONO sources increased from 11.9 % at the 90 m to 16.0 % at the 528 m.

High organic aerosol in the low layer over a rural site in the North China Plain (NCP): Observations based on large tethered balloon.

High mass concentration of organic aerosol (OA) and its fraction in PM2.5 (particle matter with radius <2.5 µm) were observed in the low layer over a rural site of the North China Plain (NCP) in winter 2018. The mass fraction of OA in PM2.5 was 65.5 % at ground level (5 m above ground), and decreased to 37.1 % in layer of 200-1000 m. In addition, there was a sharp decrease of OA at around the top of planetary boundary layer (PBL), which was distinctly different from the vertical distributions of secondary inorganic aerosols (SIA, e.g., nitrate (NO3-), ammonium (NH4+), and sulfate (SO42-)). The altitude with sharp decrease of OA was very low in the morning and evening, e.g., the sharp decrease of OA occurred at a height <50 m at nighttime on Dec. 19, while was elevated in the noon with the PBL development. Furthermore, OA at ground level exhibited a distinct diurnal variation with a night-to-day ratio of 2.3, which was much larger than those of SIA and inactive CO. All the above results indicated the extremely high OA concentration at the rural site was mainly attributed to direct emission from local sources, such as the combustion of coal and biomass for heating. The extremely high OA could be expected in vest rural areas of the NCP in winter because the farmer activities are very similar to the investigated rural site, underscoring the urgency to mitigate OA emission in rural area for improving the local as well as the regional air quality.

New positive feedback mechanism between boundary layer meteorology and secondary aerosol formation during severe haze events.

Severe haze events during which particulate matter (PM) increases quickly from tens to hundreds of microgram per cubic meter in 1-2 days frequently occur in China. Although it has been known that PM is influenced by complex interplays among emissions, meteorology, and physical and chemical processes, specific mechanisms remain elusive. Here, a new positive feedback mechanism between planetary boundary layer (PBL), relative humidity (RH), and secondary PM (SPM) formation is proposed based on a comprehensive field experiment and model simulation. The decreased PBL associated with increased PM increases RH by weakening the vertical transport of water vapor; the increased RH in turn enhances the SPM formation through heterogeneous aqueous reactions, which further enhances PM, weakens solar radiation, and decreases PBL height. This positive feedback, together with the PM-Radiation-PBL feedback, constitutes a key mechanism that links PM, radiation, PBL properties (e.g. PBL height and RH), and SPM formation, This mechanism is self-amplifying, leading to faster PM production, accumulation, and more severe haze pollution.