Affiliation:
1. College of Chemistry and Materials Science Fujian Normal University Fuzhou Fujian 350007 P. R. China.
2. College of Marine Equipment and Mechanical Engineering Key Laboratory of Energy Cleaning Utilization, Development, Cleaning Combustion and Energy Utilization Research Center of Fujian Province Jimei University Xiamen Fujian 361021
Abstract
AbstractTo improve the understanding of the oxidation of SO2 to SO3, the non‐adiabatic transition state theory (NA‐TST) coupling with the master equation (ME) method was adopted to study the kinetic characteristics of the spin‐forbidden recombination reaction SO2+O(3P) (+M)→SO3 (+M). By determining the minimum energy crossing point (MECP) of the triplet‐singlet potential energy surfaces, the high‐pressure limit (HPL), k∞=3.81×108 T0.998 e−1214/T cm3 mol−1 s−1 and the low‐pressure limit (LPL), k0=4.78×1036 T−6.38 e−4610/T cm6 mol−2 s−1 were obtained, respectively. The LPL rate constants were compared with the reported experimental data and good consistency was found. Besides, the hopping probability near the MECP was also determined. In addition, this work shows the potential application of NA‐TST/ME method to investigate the kinetics of similar spin‐forbidden reactions.
Funder
Natural Science Foundation of Fujian Province