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Open AccessArticle

Differences in Model Performance and Source Sensitivities for Sulfate Aerosol Resulting from Updates of the Aqueous- and Gas-Phase Oxidation Pathways for a Winter Pollution Episode in Tokyo, Japan

1
Central Research Institute of Electric Power Industry, Abiko, Chiba 270-1194, Japan
2
Graduate School of Maritime Sciences, Kobe University, Kobe, Hyogo 658-0022, Japan
3
National Institute for Environmental Studies, Tsukuba, Ibaraki 305-8506, Japan
*
Author to whom correspondence should be addressed.
Atmosphere 2019, 10(9), 544; https://doi.org/10.3390/atmos10090544
Received: 31 July 2019 / Revised: 9 September 2019 / Accepted: 9 September 2019 / Published: 12 September 2019
During the Japanese intercomparison study, Japan’s Study for Reference Air Quality Modeling (J-STREAM), it was found that wintertime SO42– concentrations were underestimated over Japan with the Community Multiscale Air Quality (CMAQ) modeling system. Previously, following two development phases, model performance was improved by refining the Fe- and Mn-catalyzed oxidation pathways and by including an additional aqueous-phase pathway via NO2 oxidation. In a third phase, we examined a winter haze period in December 2016, involving a gas-phase oxidation pathway whereby three stabilized Criegee intermediates (SCI) were incorporated into the model. We also included options for a kinetic mass transfer aqueous-phase calculation. According to statistical analysis, simulations compared well with hourly SO42– observations in Tokyo. Source sensitivities for four domestic emission sources (transportation, stationary combustion, fugitive VOC, and agricultural NH3) were investigated. During the haze period, contributions from other sources (overseas and volcanic emissions) dominated, while domestic sources, including transportation and fuel combustion, played a role in enhancing SO42– concentrations around Tokyo Bay. Updating the aqueous phase metal catalyzed and NO2 oxidation pathways lead to increase contribution from other sources, and the additional gas phase SCI chemistry provided a link between fugitive VOC emission and SO42– concentration via changes in O3 concentration. View Full-Text
Keywords: Community Multiscale Air Quality (CMAQ); East Asia; Tokyo; SO42–; stabilized Criegee intermediates (SCI) Community Multiscale Air Quality (CMAQ); East Asia; Tokyo; SO42–; stabilized Criegee intermediates (SCI)
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Itahashi, S.; Yamaji, K.; Chatani, S.; Hayami, H. Differences in Model Performance and Source Sensitivities for Sulfate Aerosol Resulting from Updates of the Aqueous- and Gas-Phase Oxidation Pathways for a Winter Pollution Episode in Tokyo, Japan. Atmosphere 2019, 10, 544.

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