Post-Transition State Direct Dynamics Simulations on the Ozonolysis of Catechol in an N 2 Bath and Comparison with Gas-Phase Results.

Chemical dynamics simulations on the post-transition state dynamics of ozonolysis of catechol are performed in this article using a newly developed QM + MM simulation model. The reaction is performed in a bath of N 2 molecules equilibrated at 300 K. Two bath densities, namely, 20 and 324 kg/m 3 , are considered for the simulation. The excitation temperatures of a catechol-O 3 moiety are taken as 800, 1000, and 1500 K for each density. At these new excitation temperatures, the gas-phase results are also computed to compare the results and quantify the effect of surrounding molecules on this reaction. Like the previous findings, five reaction channels are observed in the present investigation, producing CO 2 , CO, O 2 , small carboxylic acid (SCA), and H 2 O. The probabilities of these products are discussed with the role of bath densities. Results from the gas-phase simulation and density of 20 kg/m 3 are very similar, whereas results differ significantly at a higher bath density of 324 kg/m 3 . The rate constants for the unimolecular channel at each temperature and density are also calculated and reported. The QM + MM setup used here can also be used for other chemical reactions, where the solvent effect is important.