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Recent experimental findings indicate that HSO5 radicals mayplay a key role in the nucleation of atmospheric SO2 oxidationproducts. HSO5 radicals are metastable intermediates formed in theSO2 oxidation process, and their stability and lifetime are, atpresent, highly uncertain. Previous high-level computational studies havepredicted rather low stabilities for HSO5 with respect to dissociationinto SO3+HO2, and have predicted the net reaction HSO3+OH→SO3+HO2to be slightly exothermal. However, these studieshave not accounted for hydration of HSO5 or its precursor HSO3. Inthis study, we have estimated the effect of hydration on the stability andlifetime of HSO5 using the advanced quantum chemical methods CCSD(T)and G3B3. We have computed formation energies and free energies for mono-and dihydrates of OH, HSO3, HSO5, SO3 and HO2, and alsoreanalyzed the individual steps of the HSO3+O2→HSO5→SO3+HO2 reaction at a higher level of theory thanpreviously published. Our results indicate that hydration is likely tosignificantly prolong the lifetime of the HSO5 intermediate inatmospheric conditions, thus increasing the probability of reactions thatform products with more than one sulfur atom. Kinetic modeling indicatesthat these results may help explain the experimental observations that amixture of sulfur-containing products formed from SO2 oxidation by OHradicals nucleates much more effectively than sulfuric acid taken from aliquid reservoir

atmospheric chemistry and physics

Hydration increases the lifetime of HSO&amp;lt;sub&amp;gt;5&amp;lt;/sub&amp;gt; and enhances its ability to act as a nucleation precursor – a computational study