Abstract. Four extreme haze episodes occurred in October 2014 in the North China Plain (NCP). To clarify the formation mechanism of hazes in autumn, strengthened observations were conducted in Beijing from 5 October to 2 November. The meteorological parameters, satellite data, chemical compositions and optical properties of aerosols were obtained. The hazes originated from the NCP, developing in the southwest and northeast directions, with the highest concentration of PM2.5 of 469 μg m−3 in Beijing. The NCP was dominated by a weak high pressure system during the haze episode, which resulted in low surface wind speed and relatively stagnant weather. Moreover, the wind slowed down around Beijing city. The secondary aerosols NO3− was always higher than that of SO42−, which indicated the motor vehicles played a more important part in the hazes in October 2014, even though the oxidation rate from SO2 to SO42− was faster than that of NOx to NO3−. Sudden increases of the concentrations of organic matter, Cl− and BC (black carbon) before each haze episode implied that regional transport of pollutants by biomass burning was important for haze formation during autumn. A satellite map of fire points and the backward trajectories of the air masses also indicated this pollution source. The distinct decrease in the PBL (planetary boundary layer) height during four haze episodes restrained the vertical dispersion of the air pollutants. Water vapor also played a vital role in the formation of hazes by accelerating the chemical transformation of secondary pollutants, leading to hygroscopic growth of aerosols and altering the thermal balance of the atmosphere.
Nitrous acid (HONO) is a major precursor of tropospheric hydroxyl radical (OH) that accelerates the formation of secondary pollutants. The HONO sources, however, are not well understood, especially in polluted areas. Based on a comprehensive winter field campaign conducted at a rural site of the North China Plain, a box model (MCM v3.3.1) was used to simulate the daytime HONO budget and nitrate formation. We found that HONO photolysis acted as the dominant source for primary OH with a contribution of more than 92%. The observed daytime HONO could be well explained by the known sources in the model. The heterogeneous conversion of NO2 on ground surfaces and the homogeneous reaction of NO with OH were the dominant HONO sources with contributions of more than 36% and 34% to daytime HONO, respectively. The contribution from the photolysis of particle nitrate and the reactions of NO2 on aerosol surfaces were found to be negligible in clean periods (2%) and slightly higher during polluted periods (8%). The relatively high OH levels due to fast HONO photolysis at the rural site remarkably accelerated gas-phase reactions, resulting in the fast formation of nitrate as well as other secondary pollutants in the daytime.
HONO is an important precursor of OH radical and plays a key role in atmospheric chemistry, but its source and formation mechanism remain uncertain, especially during complex atmospheric pollution processes. In this study, HONO mixing ratios were measured by a custom-made instrument during a severe pollution event from 16 to 23 December 2016, at an urban area of Beijing. The measurement was divided into three periods: I (haze), II (severe haze) and III (clean), according to the levels of PM. This pollution episode was characterized by high levels of NO (75 ± 39 and 94 ± 40 ppbV during periods I and II, respectively) and HONO (up to 10.7 ppbV). During the nighttime, the average heterogeneous conversion frequency during the two haze periods were estimated to be 0.0058 and 0.0146 h, and it was not the important way to form HONO. Vehicle emissions contributed 52% (±16)% and 40% (±18)% to ambient HONO at nighttime during periods I and II. The contribution of homogeneous reaction of NO with OH should be reconsidered under high-NO conditions and could be noticeable to HONO sources during this pollution event. Furthermore, HONO was positively correlated with PM during periods I and II, suggesting a potential chemical link between HONO and haze particles.
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