Journal of Physical Chemistry A p. 3964 - 3973 (2000)
Update date:2022-08-16
Topics:
Nizkorodov, Sergey A.
Harper, Warren W.
Blackmon, Bradley W.
Nesbitt, David J.
The catalytic odd hydrogen (HOx) O3 cycle, OH + O3 → HO2 + O2 and HO2 + O3 → 2 O2 is one of the most important atmospheric processes leading to the natural destruction of atmospheric O3. This cycle is active at lower stratospheric altitudes (20-30 km, 190-230 K) in the mid-latitudes. The HOx chain reaction is estimated to be responsible for ~ 50% of the global O3 loss in the stratosphere. This makes it important to have accurate knowledge of the temperature dependent rate constants k1 and k2 for reliable modeling of atmospheric O3 phenomena. An extensive temperature dependent kinetic study of the catalytic HOx O3 cycle based on time-resolved, Doppler limited direct absorption spectroscopy of OH with a single mode (Δν = 0.0001/cm) high-resolution IR laser was presented. The sum of the two rate constants, k1 + k2, was measured at 190-315 K and can be accurately described by an Arrhenius-type expression (k1 + k2(cc/sec) = 2.26(40) x 10-12 exp[-976(50)/T]. These results agreed excellently with studies by Ravishanka et al. and Smith et al but were higher than the values currently accepted for atmospheric modeling. These studies reflected the first of such rate measurements to access the 190-230 K range relevant to kinetic modeling of O3 chain loss in the lower stratosphere.
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