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- W2011852835 endingPage "8993" @default.
- W2011852835 startingPage "8985" @default.
- W2011852835 abstract "Important mechanistic differences regarding C═C double-bond oxidation processes under ozone-limited and ozone-rich reaction conditions for cyclohexene-functionalized fused silica substrates serving as model systems for studying heterogeneous C═C double bond oxidation chemistry in the troposphere are evaluated. By using broadband vibrational sum frequency generation (SFG), we track heterogeneous ozone reactions in real time. Ozone levels span three orders of magnitude and represent environments ranging from pristine remote continental regions to highly polluted urban centers, ranging from 30 ppb to 3 ppm (from 7 × 1011 molecules cm−3 to 7 × 1013 molecules cm−3). We determine reaction rates and reactive uptake coefficients (γ values). At these tropospherically relevant ozone levels, the heterogeneous reaction rates follow a Langmuir−Hinshelwood-type mechanism. The product formation rates, which we determine as a function of ozone concentrations, are found to be half of the olefin reaction rates. This ratio is consistent with the previously proposed reaction pathway involving the breaking of one C═C double bond containing two olefinic CH moieties to form a product containing only one methyl group and one polar carbonyl moiety. Contact angle histograms show that out of a total of 60 measurements, there are about 25 more measurements with contact angles up to ten degrees below the mean recorded prior to reaction when ozone levels resemble remote continental conditions (50 ppb) than when ozone levels resemble urban conditions (1 ppm). The implication of these results are that the methyl formation pathway in heterogeneous ozonolysis may be less favorable than the carboxylic acid- and secondary ozonide-production pathway for ozone-limited conditions (i.e., in the remote continental troposphere or during urban nighttime) as opposed to ozone-rich (i.e., polluted urban atmosphere) conditions." @default.
- W2011852835 created "2016-06-24" @default.
- W2011852835 creator A5016338138 @default.
- W2011852835 creator A5030955437 @default.
- W2011852835 creator A5035731016 @default.
- W2011852835 creator A5054512446 @default.
- W2011852835 date "2009-07-10" @default.
- W2011852835 modified "2023-09-23" @default.
- W2011852835 title "Two Reactivity Modes in the Heterogeneous Cyclohexene Ozonolysis under Tropospherically Relevant Ozone-Rich and Ozone-Limited Conditions" @default.
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