Impact of the heterogeneous hydrolysis of N2O5 on chemistry and nitrate aerosol formation in the lower troposphere under photosmog conditions
Impact of the heterogeneous hydrolysis of N2O5 on chemistry and nitrate aerosol formation in the lower troposphere under photosmog conditions
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DOI：
10.1029/2002jd002436
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发表时间：
2003-02
影响因子：
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通讯作者：
N. Riemer;H. Vogel;B. Vogel;B. Schell;I. Ackermann;C. Kessler;H. Hass
中科院分区：
文献类型：
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作者：
N. Riemer;H. Vogel;B. Vogel;B. Schell;I. Ackermann;C. Kessler;H. Hass
[1]对流层气相和颗粒相化学N2O5的非均相水解的影响进行了研究，通过执行模型模拟与两个全面的模型系统，并考虑到最近的研究结果N2O5的非均相反应概率。因此，我们集中在对流层低层的光雾条件。化学箱模型运行进行忽略传输和沉积过程。N2O5的非均相水解导致在低NOx条件下臭氧的减少和在高NOx条件下臭氧的强烈增加。一维模拟进行考虑到垂直混合过程，沉积和排放的时间变化。根据模拟的气溶胶表面积密度确定的非均相水解的速率常数。结果表明，非均相水解对夜间N2O5、NO3、HNO3的浓度以及气溶胶的表面积密度和硝酸盐含量有较大影响，但N2O5水解对臭氧的影响较箱模式的影响明显减弱。三维模拟一个典型的夏季烟雾情况的西南部的德国和欧洲的规模，其中包括各种大气和排放条件，证实了这些发现。非均相水解对臭氧的影响是小的，但它会导致显着的变化，夜间浓度的含氮物种和气溶胶特性，如表面积密度和硝酸盐含量。
[1] The impact of the heterogeneous hydrolysis of N2O5 on tropospheric gas phase and particle phase chemistry was investigated by performing model simulations with two comprehensive model systems and taking into account recent findings on the heterogeneous reaction probability of N2O5. Hereby, we focused on photosmog conditions in the lower troposphere. Chemistry box model runs were carried out neglecting transport and deposition processes. The heterogeneous hydrolysis of N2O5 leads to a decrease of ozone under low-NOx conditions and to a strong increase of ozone under high-NOx conditions. One-dimensional simulations were performed to take into account vertical mixing processes, deposition, and temporal changes of the emissions. The rate constant for the heterogeneous hydrolysis was determined depending on the simulated aerosol surface area density. A large impact of the heterogeneous hydrolysis on the nocturnal concentrations of N2O5, NO3, HNO3, and the surface area density and nitrate content of the aerosol is found. However, the effect of the hydrolysis of N2O5 on ozone decreases considerably compared to the box model simulations. Three-dimensional simulations for a typical summer smog situation for the southwestern part of Germany and on the European scale, which cover a variety of atmospheric and emission conditions, confirm these findings. The impact of heterogeneous hydrolysis on ozone is small, but it causes remarkable changes in the nocturnal concentrations of nitrogen-containing species and on aerosol properties such as surface area density and nitrate content.