Study of the catalytic combustion of lean hydrogen-air mixtures in a monolith reactor

This paper presents an experimental study of catalytic hydrogen combustion that used commercial catalysts containing Pt in a honeycomb monolith reactor in a plug flow configuration. The emphasis is on determining global kinetics in the case of low hydrogen content. Measurements of the temperature and composition of the reaction product at the outlet in the steady state condition at the different initial compositions of hydrogen and total volumetric feed rates were performed. The conversion of hydrogen was determined in parallel to the composition of the reaction product at the outlet using GC as well as by means of the thermodynamic approach using material and energy balances. The influence of the flow rate and initial molar fraction of hydrogen on hydrogen conversion is shown. A kinetic expression of the Arrhenius type is proposed with the reaction first order in hydrogen and zero order in oxygen for the overall process of the oxidation of hydrogen in lean hydrogen-air mixtures. The determined activation energy was in good agreement with the desorption activation energy for O₂ from graphene-covered Pt(111) surfaces using temperature-programmed desorption. This result shows transport-limitations for heterogeneous hydrogen conversion in catalytic hydrogen combustion.