logo
    A Novel Pathway of Atmospheric Sulfate Formation Through Carbonate Radical
    Yangyang LiuYue DengJiarong LiuXiaozhong FangTao WangKejian LiKedong GongAziz-Ur-Rahim BachaIqra NabiXiuhui ZhangC. GeorgeLiwu Zhang
    0
    Citation
    0
    Reference
    10
    Related Paper
    Abstract:
    Abstract. Carbon dioxide is considered an inert gas that rarely participates in atmospheric chemical reactions. However, we show here that CO2 is involved in some important photo-oxidation reactions in the atmosphere through the formation of carbonate radicals (CO3∙-). This potentially active intermediate CO3∙- is routinely overlooked in atmospheric chemistry regarding its effect on sulfate formation. Present work demonstrates that SO2 uptake coefficient is enhanced by 17 times on mineral dust particles driven by CO3∙-. It can be produced through two routes over mineral dust surfaces: i) hydroxyl radical + CO32-; ii) holes (h+) + CO32-. Employing a suite of laboratory investigations of sulfate formation in the presence of carbonate radical on the model and authentic dust particles, field measurements of sulfate and (bi)carbonate ions within ambient PM, together with density functional theory (DFT) calculations for single electron transfer processes in terms of CO3∙--initiated S(IV) oxidation, a new role of carbonate radical in atmospheric chemistry is elucidated.
    Keywords:
    Carbonate Ion
    Inert gas
    Mineral dust
    Atmospheric chemistry
    Hydroxyl radical
    Topics:
    Atmospheric chemistry and aerosols
    Atmospheric Ozone and Climate
    Atmospheric and Environmental Gas Dynamics
    PDF
    Hydroxyl radicals in indoor environments
    Atmospheric Environment (2002)
    Golam SarwarRichard L. CorsiYosuke KimuraDavid T. AllenCharles J. Weschler
    Hydroxyl radical
    Hydroxyl value
    Citations (155)
    The effect of basic pH and carbonate ion on the mechanism of photocatalytic destruction of cylindrospermopsin
    Water Research (2015)
    Geshan ZhangXuexiang HeMallikarjuna N. NadagoudaKevin Ε. Ο'SheaDionysios D. Dionysiou
    Hydroxyl radical
    Free-radical reaction
    Carbonate Ion
    Moiety
    Citations (105)
    Quantitation of hydroxyl radical during Fenton oxidation following a single addition of iron and peroxide
    Chemosphere (2000)
    Michele E. LindseyMatthew A. Tarr
    Hydroxyl radical
    Benzoic acid
    Free-radical reaction
    Peroxide
    Radical ion
    Citations (288)
    Radiocarbon tracer measurements of atmospheric hydroxyl radical concentrations
    Journal of Atmospheric Chemistry (1986)
    M. J. CampbellJ. Carl FarmerC. A. FitznerMiguel HenryJ.C. Sheppard
    Hydroxyl radical
    TRACER
    Atmospheric chemistry
    Citations (30)
    Understanding the production and interconversion of the hydroxyl radical during the Tropospheric OH Photochemistry Experiment
    Journal of Geophysical Research Atmospheres (1997)
    F. L. EiseleG. H. MountDavid J. TannerAnne JeffersonR. E. Shetter
    The hydroxyl radical plays a critical role in the chemistry of the lower atmosphere. Understanding its production, interconversion, and sinks is central to modeling and predicting the chemistry of the troposphere. The OH measurements made during the 1993 Tropospheric OH Photochemistry Experiment provide a detailed look at these mechanisms since NO x , j (O 3 ), RO 2 , HO 2 , nonmethane hydrocarbons (NMHC), and many other relevant species were measured simultaneously. The relationship of OH to NO x and to primary production is extensively examined. Close agreement with theory is shown in the NO x /OH relation with OH concentrations increasing with increasing NO to a maximum at 1–2 ppbv due to conversion of HO 2 to OH, and then OH decreasing with further increasing NO x due to conversion of NO 2 to HNO 3 . Close correlations of OH concentrations with primary production (water, ozone, j (O 3 )) are also shown both on average and on rapid timescales.
    Hydroxyl radical
    Atmospheric chemistry
    Tropospheric ozone
    Primary (astronomy)
    Citations (64)