In this work we tackle the problem of dealing in an ab initio fashion with the description of the O(3P) + CH3OH → OH + CH2OH reaction that is one of the most important elementary processes involved in the methanol oxidation. In particular, we carried out the following computational steps: 1. calculate the electronic structure of the O + CH3OH system 2. fit to a pseudo triatomic LEPS (London Eyring Polanyi Sato) the collinear reaction channel leading to the production of OH 3. calculate the dynamical properties of the process using quantum techniques For the purpose of ab initio computing the electronic structure of the O(3P) + CH3OH system we used various computational programs based on DFT techniques (to characterize the stationary points and work out harmonic vibrational frequencies) and CCSD(T) level of theory (to refine the energy of the stationary points, calculate the exoergicity of the considered channel and estimate the height of the barrier to reaction). For the purpose of computing quantum reactive scattering state specific probabilities on the proposed LEPS potential energy surface, the Multi Configuration Time Dependent Hartree method was used.
Modeling combustions: The ab initio treatment of the O(3P) + CH3OH reaction
PACIFICI, Leonardo;BALUCANI, Nadia;FAGINAS LAGO, Maria Noelia;LAGANA', Antonio
2016
Abstract
In this work we tackle the problem of dealing in an ab initio fashion with the description of the O(3P) + CH3OH → OH + CH2OH reaction that is one of the most important elementary processes involved in the methanol oxidation. In particular, we carried out the following computational steps: 1. calculate the electronic structure of the O + CH3OH system 2. fit to a pseudo triatomic LEPS (London Eyring Polanyi Sato) the collinear reaction channel leading to the production of OH 3. calculate the dynamical properties of the process using quantum techniques For the purpose of ab initio computing the electronic structure of the O(3P) + CH3OH system we used various computational programs based on DFT techniques (to characterize the stationary points and work out harmonic vibrational frequencies) and CCSD(T) level of theory (to refine the energy of the stationary points, calculate the exoergicity of the considered channel and estimate the height of the barrier to reaction). For the purpose of computing quantum reactive scattering state specific probabilities on the proposed LEPS potential energy surface, the Multi Configuration Time Dependent Hartree method was used.I documenti in IRIS sono protetti da copyright e tutti i diritti sono riservati, salvo diversa indicazione.
