Partitioning of HNO3 and particulate nitrate over Tokyo:: Effect of vertical mixing

被引:71
作者
Morino, Y.
Kondo, Y.
Takegawa, N.
Miyazaki, Y.
Kita, K.
Komazaki, Y.
Fukuda, M.
Miyakawa, T.
Moteki, N.
Worsnop, D. R.
机构
[1] Univ Tokyo, Adv Sci & Technol Res Ctr, Meguro Ku, Tokyo 1538904, Japan
[2] Ibaraki Univ, Dept Environm Sci, Mito, Ibaraki 3108512, Japan
[3] Aerodyne Res Inc, Ctr Aerosol & Cloud Chem, Billerica, MA 01821 USA
关键词
D O I
10.1029/2005JD006887
中图分类号
P4 [大气科学(气象学)];
学科分类号
0706 ; 070601 ;
摘要
[ 1] Ground-based measurements of gas-phase nitric acid (HNO3) and particulate nitrate (NO3-) were performed in Tokyo during 2003 - 2004. These measurements provide a comprehensive data set for investigating the diurnal and seasonal variations of gas-phase HNO3 and particulate NO3- and the thermodynamic equilibrium of these compounds. HNO3 and NO3- have distinct diurnal and seasonal variations, especially in summer. This study shows that the thermodynamic equilibrium of HNO3 and NO3- and the production rate of total nitrate (TNO3 = HNO3 + NO3-) are the major controlling factors affecting these seasonal and diurnal variations. A thermodynamic equilibrium model (ISORROPIA) is newly coupled with a one-dimensional (1-D) model to take into account the effect of vertical mixing during daytime on the partitioning of HNO3 and NO3- by constraining the TNO3 concentrations to the observations. The 1-D model reproduces the NO3-/TNO3 ratios observed during daytime, whereas the equilibrium model significantly underestimates these ratios. The agreement between the observed and calculated NO3-/TNO3 ratios is improved over the observed temperature range (1 degrees- 34 degrees C) and relative humidity (18 - 95%) by the 1-D model. These results suggest the importance of vertical mixing in determining HNO3-NO3- partitioning in the boundary layer. It is also found that the mass accommodation coefficient for HNO3 needs to be approximately 0.1 to explain the observed HNO3-NO3- partitioning at the surface.
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页数:19
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