Elementary-step based kinetic modeling using KASTER: a top-down approach
applied to methane steam reforming
Abstract
A top-down kinetic modeling methodology is proposed using the in-house
developed software tool ‘KASTER’. As a case study, it is applied in the
assessment of methane steam reforming (MSR) kinetics on a Ni catalyst,
including water-gas shift (WGS) as a side-reaction. The complexity of
the reaction mechanism is gradually enhanced, leading ultimately, to a
microkinetic model. The reactor equations are solved in a transient
manner, preventing the crucial numerical challenges encountered in the
steady-state solution. The model providing the best balance between
detail and significance was found to be of the
Langmuir-Hinshelwood-Hougen-Watson (LHHW) type accounting for
dissociative adsorption. In this model, the rate-determining steps of
MSR and WGS are CO formation and COOH formation, respectively. While the
microkinetic variant indicated that both CH4
dissociative adsorption and CO formation are kinetically relevant steps
in MSR, CO formation is found to be rate determining at 923 K using the
adopted methodology.