Reactive and nonreactive quenching of O(1D) by the potent greenhouse gases SO2F2, NF3, and SF5CF3
作者： Z. Zhao , P. L. Laine , J. M. Nicovich , P. H. Wine
关键词: Global-warming potential 、 Arrhenius equation 、 Quenching rate 、 Photochemistry 、 Analytical chemistry 、 Ozone 、 Molecule 、 Fluorescence 、 Chemistry 、 Ozone chemistry 、 Kinetics
摘要: A laser flash photolysis-resonance fluorescence technique has been employed to measure rate coefficients and physical vs. reactive quenching branching ratios for O((1)D) deactivation by three potent greenhouse gases, SO(2)F(2)(k(1)), NF(3)(k(2)), SF(5)CF(3)(k(3)). In excellent agreement with one published study, we find that k(1)(T) = 9.0 x 10(-11) exp(+98/T) cm(3) molecule(-1) s(-1) the coefficient is k(1b) (5.8 +/- 2.3) independent of temperature. We k(2)(T) 2.0 exp(+52/T) reaction proceeding almost entirely (approximately 99%) quenching. Reactive NF(3) more than a factor two faster reported in result will significantly lower model-derived atmospheric lifetime global warming potential NF(3). Deactivation SF(5)CF(3) slow enough (k(3) < 10(-13) at 298 K) unimportant as an removal mechanism SF(5)CF(3). The kinetics reactions SO(2) (k(4)) CS(2) (k(5)) have also investigated K. k(4) (2.2 0.3) 10(-10) k(5) (4.6 0.6) s(-1); are 0.76 0.12 0.94 0.06 reactions, respectively. All uncertainties above estimates accuracy (2sigma) k(i)(T) (i 1,2) calculated from Arrhenius expressions estimated accuracies 15% (2sigma).
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