Combination of Langmuir-Hinshelwood-Hougen-Watson and microkinetic approaches for simulation of biogas dry reforming over a platinum-rhodium alumina catalyst
2017
Abstract Dry reforming of CH 4 on a platinum-rhodium alumina catalyst is selected to numerically investigate biogas reforming process. Langmuir-Hinshelwood-Hougen-Watson (LHHW) rate expressions for dry reforming and reverse water-gas shift reactions are presented. Activation energies are estimated by combining microkinetics with the theory of unity bond index-quadratic exponential potential (UBI-QEP). Pre-exponential factors are initially obtained by using the transition state theory (TST) and optimised, later, by minimising errors between modelling and experimental data. Adsorption of CH 4 on the catalyst surface is found to be the rate determining step in the range of relatively low temperature (600–770 °C), while at relatively high temperature (770–950 °C) the thermal cracking of adsorbed CH 4 is the rate controlling step. Small effect of reverse water-gas shift reaction results in the ratio of H 2 to CO produced less than unity for all operating conditions. The simulation shows that the dry reforming process proceeds with reaction rate far from equilibrium state. The presented mechanism is capable of predicting the dependence of biogas dry reforming activities (e.g., reactant conversions, product formations, H 2 to CO ratio, and temperature profile inside the catalyst) on operating conditions (e.g., inlet temperature, heat supplied through the catalyst wall, and composition of biogas at inlet).
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