No abstract

Emissions from vehicles contain a variety of pollutants that must be either oxidized or reduced efficiently in the catalytic converter. Improvements to the catalyst require knowledge of the microkinetics, but the complexity of the exhaust gas mixture makes it challenging to identify the reaction network. This complexity was tackled by using the “Reaction Mechanism Generator” (RMG) to automatically generate microkinetic models for the oxidation of combustion byproducts from stoichiometric gasoline direct injection engines on Pt(111). The possibilities and the limitations encountered during the generation procedure are discussed in detail. A combination of first-principles-based mechanism construction and top-down parameter refinement allows a description of experimental results obtained by kinetic testing of a Pt/Al2O3 monolith under stoichiometric conditions. The study can serve as a blueprint for the usage of RMG for other challenging heterogeneously catalyzed reactions.

No abstract

No abstract

 Ni and Rh on La2O3-CeO2-ZrO2 low temperature CH4 steam reforming kinetics studied  Kinetic isotope effects during CH4 steam reforming and decomposition measured  C-H bond activation kinetically limiting over Ni and Rh with no steam participation  Microkinetic modelling identifies CH3* dehydrogenation as the rate determining step  Binding energies of key surface species help discriminate catalysts' performance