Transient behaviour of perovskite-based monolithic reactors in the catalytic combustion of methane

Abstract

The transient behaviour of perovskite-based catalysts prepared via active phase dispersion on La/γ-Al2O3 washcoated cordierite monoliths has been investigated in the autothermal combustion of lean methane mixtures. During start-up and shut-down operations, the reaction front moves from the outlet towards the inlet (ignition) or vice versa (extinction), with a time scale significantly higher than space time. The CH4/O2/N2 feed mixture is completely converted to CO2 and H2O provided its inlet temperature is about 500°C, a value not affected by catalyst length and gas flow rate, the phenomenon being kinetically controlled. Gas flow rate significantly affects solid steady-state temperature, as at higher flow rates the thermal power produced by combustion is higher in comparison with heat losses by radiation and conduction and temperature rise is closer to the adiabatic value. The fresh catalysts weakly deactivate during the first 60h of operation under reaction conditions, but after 120h the activity is still very high and not significantly affected by further ageing. The transient behaviour of the system has been simulated by a mathematical model, characterised by an increased solid thermal conductivity to take into account the relevant contribution of internal radiation between channel surfaces.