Trends and outlook of computational chemistry and microkinetic modeling for catalytic synthesis of methanol and DME

Abstract

The first-principle modeling of heterogeneous catalysts is a revolutionarily approach, as the electronic structure of a catalyst is closely related to its reactivity on the surface with reactant molecules. In the past, detailed reaction mechanisms could not be understood, however, computational chemistry has made it possible to analyze a specific elementary reaction of a reaction system. Microkinetic modeling is a powerful tool for investigating elementary reactions and reaction mechanisms for kinetics. Using a microkinetic model, the dominant pathways and rate-determining steps can be elucidated among the competitive reactions, and the effects of operating conditions on the reaction mechanisms can be determined. Therefore, the combination of computational chemistry and microkinetic modeling can significantly improve computational catalysis research. In this study, we reviewed the trends and outlook of this combination technique as applied to the catalytic synthesis of methanol (MeOH) and dimethyl ether (DME), whose detailed mechanisms are still controversial. Although the scope is limited to the catalytic synthesis of limited species, this study is expected to provide a foundation for future works in the field of catalysis research based on computational catalysis.