Thermal sintering studies of an autothermal reforming catalyst

Abstract

This paper describes a novel approach to life studies on catalysts used in non-isothermal reactors, using a single long-term experiment. Temperature dependence of catalyst aging is determined by comparing the activity reduction of portions of the catalyst from different sections of the reactor, subjected to different temperatures. Time dependence is determined by fitting the drift in catalyst temperatures to a time-dependent reaction rate via a thermodynamic reactor model. Experimentally, a monolithic autothermal reforming catalyst was subjected to thermally accelerated aging under reforming conditions in an adiabatic laboratory mini-flow reactor for 1000h. Methane was used as the fuel. The axial temperature profile of the catalyst was monitored using thermocouples placed at various locations along the catalyst. A gradual change in temperature profile, with increasing temperatures due to decreasing steam-reforming activity, was observed. The aged monolith was cut up into short pieces centered on the thermocouple locations. The pieces, each aged at a different temperature due to its location, were tested individually for activity. The reduced activities were correlated with the aging temperature to obtain the temperature dependence of thermal sintering rates. A generalized power-law equation (GPLE) model for sintering was fit to the activity data. A plug flow reactor (PFR) model describing the reaction was built and the sintering kinetics were incorporated. The PFR model was used to predict changes in catalyst performance due to sintering under normal operating conditions. Thermal sintering deactivation for this catalyst was found to be within acceptable limits for commercial applications.