Abstract
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 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.
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