Atmospheric Behavior of Nitrous Acid and Nitrogen Dioxide in Northern Japan

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  • 北日本における亜硝酸ガス濃度と窒素酸化物由来成分の挙動
  • キタニホン ニ オケル アショウサン ガス ノウド ト チッソ サンカブツ ユライ セイブン ノ キョドウ

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Abstract

The atmospheric behavior of nitrous acid, HONO, was discussed on the basis of field measurements by an annular-denuder or a filter-pack method at four different nature sites in northern Japan, Sapporo (urban), Moshiri (rural), Rishiri (coastal remote) and Teshio (mountainous remote), in terms of their atmospheric chemistry parameters including nitrogen oxides, nitric acid, nitrate aerosol and ozone. The annual mean concentrations of HONO in Sapporo ranged from 36 to 41 nmol m-3 where the concentration level was 11 to 31 times higher than those for the other sites. A different seasonality of the HONO concentration was detected at the different nature site: the urban site showed a maximum in the winter, the remote in the summer, and the rural in the winter and the summer. A heterogeneous reaction between NO2 and H2O on the surface of airborne particles and the ground surface is likely to play a significant role in the nitrous acid formation because the HONO/NOx ratio in ambient air is higher than those by direct emission as reported by Kurtenbach et al. (2001). In the case of the ground-surface heterogeneous reaction, the concentration gradient of HONO is expected to negative correlate with that of NO2 because the deposition of NO2 would induce emissions of HONO into the atmosphere. Actually, in Teshio, the difference between the concentrations of HONO at the heights of 30 m and 10 m positive correlated with that for NO2. Furthermore, the Rishiri measurements showed a significant correlation between the concentrations of HONO and PM10. In addition, Rishiri and Moshiri measurements showed significant correlations between the concentration ratio, HONO/NO2, and absolute humidity. These results strongly support the view that the heterogeneous reactions on the airborne particles prevails in the formation of HONO in the rural and remote areas with considerably low concentrations of NO2. On the other hand, the heterogeneous reaction on the ground-surface reaction plays a significant role in Sapporo, especially in the winter with high NO2 concentrations. In Sapporo, negative correlations were detected in the winter between the concentrations of HONO and NO, and between of HNO3 and O3, which would be attributable to the insufficient conversion of NO2 to HNO3, and further to nitrate species, under urban conditions because of the low concentration of ozone along with high concentrations of NO. These field measurements would indicate that the behavior of nitrous acid is controlled by the chemical reactions of NO2 with H2O, and that this heterogeneous reaction was affected by the NO2 concentration, absolute humidity and O3 concentration.

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