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. Atmospheric models often underestimate particulate sulfate, a majorcomponent in ambient aerosol, suggesting missing sulfate formationmechanisms in the models. Heterogeneous reactions between SO2 andaerosol play an important role in particulate sulfate formation and itsphysicochemical evolution. Here we study the reactive uptake kinetics ofSO2 onto aerosol containing organic peroxides. We present chamberstudies of SO2 reactive uptake performed under different relativehumidity (RH), particulate peroxide contents, peroxide types, and aerosolacidities. Using different model organic peroxides mixed with ammoniumsulfate particles, the SO2 uptake coefficient (γSO2) wasfound to be exponentially dependent on RH. γSO2 increasesfrom 10−3 at RH 25 % to 10−2 at RH 71 % as measured for anorganic peroxide with multiple O–O groups. Under similar conditions, thekinetics in this study were found to be structurally dependent: organicperoxides with multiple peroxide groups have a higher γSO2 thanthose with only one peroxide group, consistent with the reactivity trendpreviously observed in the aqueous phase. In addition, γSO2 is linearly related to particle-phase peroxide content, which in turndepends on gas–particle partitioning of organic peroxides. Aerosol acidityplays a complex role in determining SO2 uptake rate, influenced bythe effective Henry's Law constant of SO2 and the condensed-phasekinetics of the peroxide–SO2 reaction in the highly concentratedaerosol phase. These uptake coefficients are consistently higher than thosecalculated from the reaction kinetics in the bulk aqueous phase, and we showexperimental evidence suggesting that other factors, such as particle-phaseionic strength, can play an essential role in determining the uptakekinetics. γSO2 values for different types of secondary organicaerosol (SOA) were measured to be on the order of 10−4. Overall, thisstudy provides quantitative evidence of the multiphase reactions betweenSO2 and organic peroxides, highlighting the important factors thatgovern the uptake kinetics.

Heterogeneous interactions between SO&lt;sub&gt;2&lt;/sub&gt; and organic peroxides in submicron aerosol

Heterogeneous interactions between SO<sub>2</sub> and organic peroxides in submicron aerosol