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

The transient behaviour of perovskite-based catalysts prepared via active p hase dispersion on La/gamma -Al2O3 washcoated. cordierite monoliths has bee n investigated in the autothermal combustion of lean methane mixtures. Duri ng start-up and shut-down operations, the reaction front moves from the out let towards the inlet (ignition) or vice versa (extinction), with a time sc ale significantly higher than space time. The CH4/O-2/N-2 feed mixture is c ompletely converted to CO2 and H2O provided its inlet temperature is about 500 degreesC, a value not affected by catalyst length and gas flow rate, th e phenomenon being kinetically controlled. Gas flow rate significantly affe cts solid steady-state temperature, as at higher flow rates the thermal pow er produced by combustion is higher in comparison with heat losses by radia tion and conduction and temperature rise is closer to the adiabatic value. The fresh catalysts weakly deactivate during the first 60 h of operation un der reaction conditions, but after 120 h the activity is still very high an d 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 cont ribution of internal radiation between channel surfaces. (C) 2001 Elsevier Science B.V. All rights reserved.