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Title: Investigation of OH dynamics in the argon sensitized pulse radiolysis of water vapor

Journal Article · · J. Appl. Phys.; (United States)
DOI:https://doi.org/10.1063/1.337217· OSTI ID:5501812

Reactions of OH radical were studied in systems containing 650-Torr Ar and from 0.5 to 9-Torr H/sub 2/O using the method of pulse radiolysis-absorption spectroscopy. It was found that initial concentrations of OH radical increased and the half-life for its loss decreased at higher water pressures. Dependence of OH half-life on OH concentrations occurs because homogeneous OH loss processes are second order in reaction intermediates, whose concentration increases with added H/sub 2/O. A contribution by water in chaperoning OH/OH and OH/H combination is also important. The kinetic scheme was examined with a Gear integrator. A good fit of the experimental rate data was obtained using literature values for rate constants of OH+OH, OH+H, and H+H reactions, when experimental zero-time absorbance values were converted to OH concentrations based on an extinction coefficient of 6.37 x 10/sup 4/ l mol/sup -1/ cm/sup -1/ at 309.5 nm. Using the same extinction coefficient, an alternative empirical reduction of rate data gives k-italic (apparent bimolecular) for loss of OH at 650-Torr Ar pressure of 5.06 x 10/sup -11/ cm/sup 3/ molec/sup -1/ s/sup -1/, consistent with literature rate constants within 10%. Dependence of OH yield on water concentration is interpreted on a two state model for argon precursor, involving short-lived (resonance state) Ar* (/sup 1/P-italic/sub 1/ and /sup 3/P-italic/sub 1/) and longer-lived (metastable) Ar** (/sup 3/P-italic/sub 2/ and /sup 3/P-italic/sub 0/). Adjustment of assumed initial Ar* and Ar** concentrations allowed prediction of measured OH concentrations within experimental error at all water pressures studied.

Research Organization:
Department of Chemistry, University of Florida, Gainesville, Florida 32611
OSTI ID:
5501812
Journal Information:
J. Appl. Phys.; (United States), Vol. 60:6
Country of Publication:
United States
Language:
English