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The kinetics of the reaction OH/OD(v = 1,2,3) + SO 2 were studied using a photolysis/laser-induced fluorescence technique. The rate coefficients OH/OD(v = 1,2,3) + SO 2 , k 1 , over the temperature range of 295-810 K were used to determine the limiting high-pressure limit k 1  ∞ . This method is usually applicable if the reaction samples the potential well of the adduct HOSO 2 and if intramolecular vibrational relaxation is fast. In the present case, however, the rate coefficients showed an additional fast removal contribution as evidenced by the increase in k 1 with vibrational level; this behavior together with its temperature dependence is consistent with the existence of a weakly bound complex on the potential energy surface prior to adduct formation. The data were analyzed using a composite mechanism that incoporates energy-transfer mechanisms via both the adduct and the complex, and yielded a value of k 1  ∞ (295 K) equal to (7.2 ± 3.3) × 10 -13 cm 3 molecule -1 s -1 (errors at 1σ), a factor of between 2 and 3 smaller than the current recommended IUPAC and JPL values of (2.0 -1.0  +2.0 ) and (1.6 ± 0.4) × 10 -12 cm 3 molecule -1 s -1 at 298 K, respectively, although the error bars do overlap. k 1  ∞ was observed to only depend weakly on temperature. Further evidence for a smaller k 1  ∞ is presented in the companion paper.

the journal of physical chemistry a

An Experimental Study of the Kinetics of OH/OD(<i>v</i> = 1,2,3) + SO<sub>2</sub>: The Limiting High-Pressure Rate Coefficients as a Function of Temperature

An Experimental Study of the Kinetics of OH/OD(v = 1,2,3) + SO2: The Limiting High-Pressure Rate Coefficients as a Function of Temperature

An Experimental Study of the Kinetics of OH/OD(v = 1,2,3) + SO₂: The Limiting High-Pressure Rate Coefficients as a Function of Temperature