Autothermal Reforming of Methane on Rhodium Catalysts: Microkinetic Analysis for Model Reduction

摘要

Methane autothermal reforming has been studied using comprehensive, detailedmicrokinetic mechanisms, and a hierarchically reduced rate expression has beenderived without apriori assumptions. The microkinetic mechanism is adapted fromliterature and has been validated with reported experimental results. RateDetermining Steps are elicited by reaction path analysis, partial equilibriumanalysis and sensitivity analysis. Results show that methane activation occursvia dissociative adsorption to pyrolysis, while oxidation of the carbon occursby O(s). Further, the mechanism is reduced through information obtained fromthe reaction path analysis, which is further substantiated by principalcomponent analysis. A 33% reduction from the full microkinetic mechanism isobtained. One-step rate equation is further derived from the reducedmicrokinetic mechanism. The results show that the this rate equation accuratelypredicts conversions as well as outlet mole fraction for a wide range of inletcompositions.