Development of a methodology for determining reaction pathways and rate constants of complex combustion networks

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In many chemical and combustion engineering applications, chemical reaction mechanisms are required to model and optimize processes and devices accurately. Due to the large number of reactions and species, often the determination of rate coefficients of all elementary reactions is not possible from experimentally accessible data. Therefore, experiments have been augmented by ab initio calculations in the last years. Such calculations, however, require much chemical intuition, large amounts of human and computer time, and still their accuracy sometimes suffers from the simplifications made in the models used. In this work, we suggest to overcome these issues by performing molecular dynamics simulations with a reactive force field to automatically identify reaction paths and transition states. The latter ones will be refined in an automated procedure by quantum mechanics and used to compute reaction rates. Molecular simulations can also be used to relax some of the assumptions made in the transition state theory models usually used. Therefore, we expect to develop a methodology that will allow the determination of reaction models more efficiently and with higher accuracy than it is presently possible. This methodology will be used to investigate the ignition properties and the formation of pollutants of novel biofuels.