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Hoffmann, R. A wiki for the life sciences where authorship matters. Nature Genetics (2008)
 
 
 

Kinetics of OH radical reaction with anthracene and anthracene-d10.

Using a refined pulsed laser photolysis/pulsed laser-induced fluorescence ( PLP/PLIF) technique, the kinetics of the reaction of a surrogate three-ring polynuclear aromatic hydrocarbons (PAH), anthracene (and its deuterated form), with hydroxyl (OH) radicals was investigated over the temperature range of 373 to 1200 K. This study represents the first examination of the OH kinetics for this class of reactions at elevated temperatures (>470 K). The results indicate a complex temperature dependence similar to that observed for simpler aromatic compounds, e.g., benzene. At low temperatures (373-498 K), the rate measurements exhibited Arrhenius behavior (k = 1.82 x 10(-11) exp(542.35/T) in units of cm3 molecule(-1) s(-1)), and the kinetic isotope effect (KIE) measurements were consistent with an OH-addition mechanism. The low-temperature results are extrapolated to atmospheric temperatures and compared with previous measurements. Rate measurements between 673 and 923 K exhibited a sharp decrease in the magnitude of the rate coefficients (a factor of 9). KIE measurements under these conditions were still consistent with an OH-addition mechanism. The following modified Arrhenius equation is the best fit to our anthracene measurements between 373 and 923 K (in units of cm3 molecule(-1) s(-1)): k(1) (373-923 K) = 8.17 x 10(14) T(-8.3) exp(-3171.71/T). For a limited temperature range between 1000 and 1200 K, the rate measurements exhibited an apparent positive temperature dependence with the following Arrhenius equation, the best fit to the data (in units of cm3 molecule(-1) s(-1)): k1 (999-1200 K) = 2.18 x 10(-11) exp(-1734.11/T). KIE measurements above 999 K were slightly larger than unity but inclusive regarding the mechanism of the reaction. Theoretical calculations of the KIE indicate the mechanism of reaction at these elevated temperatures is dominated by OH addition with H abstraction being a minor contributor.[1]

References

  1. Kinetics of OH radical reaction with anthracene and anthracene-d10. Ananthula, R., Yamada, T., Taylor, P.H. The journal of physical chemistry. A, Molecules, spectroscopy, kinetics, environment & general theory. (2006) [Pubmed]
 
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