Nitrate (NO3−), which is mainly oxidized from NO2 by the OH radical (OH·) and O3 in the atmosphere, is a major component of inorganic aerosols. However, the contributions of the OH· and O3 pathways to NO3− in urban aerosols and the influence of air pollution to both pathways remain unclear. Oxygen isotopes of NO3− were measured for PM2.5 in Beijing in 2014. The Δ17O‐NO3− values (17.0–32.8‰) were significantly higher in winter (27.2 ± 3.6‰) than in summer (24.2 ± 1.3‰). By estimating contributions of O3 to the NOx cycle, the Δ17O values of NO3− endmembers produced via the NO2 + OH· (P1), NO3· + DMS/HC (P2), and N2O5 hydrolysis (P3) pathways were calculated for each observation. The contributions of the three pathways (P1: 32 ± 10%, P2: 34 ± 10%, and P3: 34 ± 20% annually) were calculated using the Stable Isotope Analysis in R model. We found that NO3− formation was dominated by the O3 oxidation pathways (P2 + P3; 68 ± 23% annually, 73 ± 21% in spring, 59 ± 23% in summer, 75 ± 20% in autumn, and 69 ± 22% in winter). Moreover, PM2.5, NO2, and NO3− pollution decreased the importance of the OH· pathway relative to the O3 pathways for NO3− production. However, O3 pollution increased the importance of the OH· pathway relative to the O3 pathways for NO3− production. These results provided a comprehensive analysis on the oxygen isotope records in particulate NO3− for understanding the relative importance of major oxidation pathways of NO2. Atmospheric pollution substantially influenced the pathways of NO2 oxidation to NO3− in city environments.
Abstract. The real-time measurements of NH 3 and trace gases were conducted, in conjunction with semi-continuous measurements of water-soluble ions in PM 2.5 at a rural site in the North China Plain (NCP) from May to September 2013 in order to better understand chemical characteristics of ammonia and the impact of secondary ammonium aerosols on formation in the NCP. Extremely high NH 3 and NH + 4 concentrations were observed after a precipitation event within 7-10 days following urea application. Elevated NH 3 levels coincided with elevated NH + 4 , indicating that NH 3 likely influenced particulate ammonium mass. For the sampling period, the average conversion / oxidation ratios for NH + 4 (NHR), SO 2− 4 (SOR), and NO − 3 (NOR) were estimated to be 0.30, 0.64, and 0.24, respectively. The increased NH 3 concentrations, mainly from agricultural activities and regional transport, coincided with the prevailing meteorological conditions. The high NH 3 level with NHR of about 0.30 indicates that the emission of NH 3 in the NCP is much higher than needed for aerosol acid neutralisation, and NH 3 plays an important role in the formation of secondary aerosols as a key neutraliser. The hourly data obtained were used to investigate gas-aerosol partitioning characteristics using the thermody-
Abstract. The study of atmospheric nitrous acid (HONO), which is the primary source of OH radicals, is crucial with respect to understanding atmospheric photochemistry and heterogeneous chemical processes. Heterogeneous NO2 chemistry under haze conditions has been identified as one of the missing sources of HONO on the North China Plain, and also produces sulfate and nitrate. However, controversy exists regarding the various proposed HONO production mechanisms, mainly regarding whether SO2 directly takes part in the HONO production process and what roles NH3 and the pH value play. In this paper, never before seen explosive HONO production was reported and evidence was found – for the first time in field measurements during fog (usually with 4< pH <6) and haze episodes under high relative humidity (pH ≈4) – that NH3 was the key factor that promoted the hydrolysis of NO2, leading to the explosive growth of HONO and nitrate under both high and relatively lower pH conditions. The results also suggest that SO2 plays a minor or insignificant role in HONO formation during fog and haze events, but was indirectly oxidized upon the photolysis of HONO via subsequent radical mechanisms. Aerosol hygroscopicity significantly increased with rapid inorganic secondary aerosol formation, further promoting HONO production as a positive feedback. For future photochemical and aerosol pollution abatement, it is crucial to introduce effective NH3 emission control measures, as NH3-promoted NO2 hydrolysis is a large daytime HONO source, releasing large amounts of OH radicals upon photolysis, which will contribute largely to both atmospheric photochemistry and secondary aerosol formation.
The distribution of organochlorine pesticides and polychlorinated biphenyls in air along an altitudinal transect on Balang Mountain in western China was measured by deploying XAD-2 resin based passive air samplers in duplicate at seven sites with elevations ranging from 1242 to 4485 m above sea level for five consecutive six-month periods between 2005 and 2008. Analyzed by gas chromatography-high resolution mass spectrometry, concentrations of hexachlorobenzene were highest, followed by hexachlorocyclohexanes, DDT-related compounds and PCB congeners 28 and 52. Except for hexachlorobenzene, which had largely uniform concentrations in space and time, there were clear seasonal variations with concentrations in summer being higher than in winter. With a few exceptions, concentrations that vary little with altitude suggest that the presence of these chemicals in the area is almost entirely due to atmospheric transport, most likely from the Chengdu plain. This is supported by similarities in the relative abundance of different compounds and in the differences between summer and winter concentrations measured in the city of Chengdu and in the mountains. Furthermore, air mass trajectories during the sampling period often originate to the East, passing over the Western part of the Sichuan basin, including the Chengdu plain, prior to arriving at the sampling sites. Higher summer time values in the mountains are due to more contaminated air being blown into the region, presumably due either to higher pesticide usage in summer or due to higher temperatures leading to higher evaporation in source regions. Air and soil from the region are in equilibrium with respect to alpha-HCH, gamma-HCH, and HCB, whereas a situation of net deposition prevails for p,p'-DDE and p,p'-DDT.
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