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Chemical Characteristics of Cloud Water and Sulfate Production Under Excess Hydrogen Peroxide in a High Mountainous Region of Central Japan
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Chemical Characteristics of Cloud Water and Sulfate Production Under Excess Hydrogen Peroxide in a High Mountainous Region of Central Japan
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Journal Article
Chemical Characteristics of Cloud Water and Sulfate Production Under Excess Hydrogen Peroxide in a High Mountainous Region of Central Japan
2021
Overview
Over the last two decades, atmospheric sulfur dioxide (SO2) concentrations have decreased in air-polluted regions. However, this decrease was accompanied by a rise in cloud water acidity (pH), which remains below 5. With this change, gas-phase hydrogen peroxide (H2O2) exceeded SO2 in most of these regions. These conditions where SO2 < H2O2 occurred at Mt. Norikura (2770 m.a.s.l.) during the 1900s. Therefore, to reveal the aqueous-phase oxidation of SO2 by H2O2, the present study investigated the inorganic and organic major ions and Se concentrations in cloud water in addition to aerosols and concentrations of gas species including O3, NOx, and SO2 collected in cloud events at Mt. Norikura during the summer of 1999. Backward air trajectory analyses indicated that the (NH4)2SO4 and trace (NH4)HSO4 aerosols originated from industrial and metropolitan areas in southwest Japan. The cloud water pH was between 3.6 and 4.4. The aqueous-phase SO42−/NO3− ratio (1.2 ± 0.6) was lower than that of the early 1990s (2.2) and 1960s (> 10) in our observation site, which was due to power plant restrictions in Japan since the 1970s. The ion species concentrations in cloud water indicated that cloud acidification resulted from dissolution of gaseous HNO3 and SO2, whereas gaseous hydrochloric acid and organic acid had a minor contribution to the acidification. Significant losses of Cl− and Mg2+ were observed in some of the cloud water. The excess value of non-sea-salt sulfate (nss-SO42−) over NH4+ in cloud water implies the in-cloud oxidation of gaseous SO2 to aqueous SO42−. A Se tracer technique was used to conduct in-situ measurements of in-cloud SO42− production. The results showed that the in-cloud production varied in a range between 7 ± 2 and 41 ± 14%. This temporal variation might be due to ambient SO2 concentrations based on Henry’s law.
