Toward the Mechanism Study of Pd/γ-Al2O3-Assisted Bioalcohol Combustion in a Flow Reactor

The combustion and catalytic combustion of ethanol (a typical bioalcohol) at atmospheric pressure and an equivalence ratio of phi = 3 were investigated in a flow reactor. Reactants, important intermediates, and products were detected and identified by gas chromatography-mass spectrometry. For ethanol combustion, the hydrogen abstraction reaction attacked by OH radicals is the initial pathway for ethanol consumption. Acetaldehyde is regarded as an important intermediate in ethanol combustion through kinetic analysis. However, catalytic combustion of ethanol over gamma-Al2O3 is dominated by bimolecular and unimolecular dehydration reactions to produce diethyl ether and C2H4 , while Pd/gamma-Al2O3 can strongly oxidize ethanol to CO2 with a dramatic decrease in the decomposition temperature. To further understand the mechanism of catalytic combustion, pyrolysis and catalytic pyrolysis of ethanol were also explored. The product distribution in catalytic pyrolysis demonstrated weaker coke deposition over gamma-Al2O3 in comparison to catalytic combustion. In addition, the deactivation of Pd/gamma-Al2O3 at high temperatures was probably due to the increase in the concentration of oxygenated species to cover the active Pd site. The apparent activation energy was estimated by the Arrhenius equation to illustrate the difference in primary reaction channels. This work bridges the gap between combustion and catalytic combustion of ethanol, which is beneficial for the improvement of catalytic performance and control of pollutants by combining pyrolysis and combustion.