Characteristics of Raindrop Acidification by Co-Washout of SO2(G)-H2O2(G)-HNO3(G)     

Watanabe  Keiichi  Shiba  Sadataka  Hirata  Yushi 《Water, air, and soil pollution》2001,130(1-4):313-318

In order to investigate the acid rain formation under the coexistence of SO₂(g), H₂O₂(g), and HNO₃(g) in the air, a mathematical model has been built and some numerical simulations have been carried out with use of the model. The simulation reveals that SO₂(g) absorbed into a raindrop is released and then re-absorbed as the fall distance increases. The desorption and re-absorption processes of SO₂(g) are caused by: (1) the fact that the equilibrium concentration of H₂O₂(aq) and HNO₃(aq) in raindrops are much higher than that of SO₂(aq), and (2) the fact that the oxidation reaction rate of HSO₃ ^? with H₂O₂(aq) increases with H⁺ concentration in raindrops. The degree of acidification of the rainwater has been estimated by introducing a raindrop size distribution. The acidification is mainly caused by the adsorption of SO₂(g) in the usual case where the atmospheric concentration of SO₂(g) is much higher than that of HNO₃(g). With the increase in the atmospheric concentration of HNO₃(g), the concentration of H⁺ generated from SO₂(g) decreases and the contribution of HNO₃(g) to the generation of H⁺ becomes dominant.

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Acidification of Growing Cloud Droplet by Rainout of SO2(g)     

Shiba  Sadataka  Hirata  Yushi  Yagi  Shunsaku 《Water, air, and soil pollution》2001,130(1-4):307-312

Growing cloud droplets absorb such atmospheric gaseous pollutant as SO₂(g), condensing atmospheric water vapor into themselves. Then, the cloud droplets are acidified by absorption of SO₂(g) during condensational growth on cloud condensation nuclei (CCN). Characteristics of this process, which is a part of rainout, have not been made clear yet. In order to estimate the contribution of rainout to acid rain formation, the acidification of growing cloud droplets is investigated numerically, using a mathematical model. The numerical simulations show that: (1) the time to attain the equilibrium state for mass transfer (acidity and growth) and heat transfer (temperature) is much longer than the time for disappearance of CCN; (2) time variation of acidity and temperature of cloud droplets are greatly dependent on the existence of undissolved CCN; and (3) there seems to be a close correlation between the time variation of the acidity and that of the temperature.  相似文献