Automated Discovery of Complex Reaction Networks: Reaction Topology, Thermochemistry and Kinetics
Shaohui Zheng, Walter Pfaendtner · 2015
Abstract : Understanding the combustion mechanism of jet fuel is essential for the design of stable, responsive, and highly efficient military jet engines. However, this is a challenging mission because of extreme conditions such as high temperature, supersonic incoming airflow, short lifetime of intermediates, the complexity of combustion reaction networks, and the difficulty to identify important reaction channels in combustion chemistry. In the present work, a physics-based approach (i.e., ab initio dynamics) was utilized to guide the enumeration and characterization of chemical reaction networks in combustion, minimize human input, and avoid on-the -fly thermochemical estimation. Based on the enumerated elementary reactions, a framework that is able to automatically reduce negligible species and elementary reactions was suggested and hence optimized reaction networks were generated. The methodology was applied to study methanol oxidation, prediction of ethylene combustion mechanism and transition states of different types of chemical reactions.