Reaction Kinetics and Mechanism of VOCs Combustion on Mn-Ce-SBA-15

Abstract

A propane combustion catalyst based on Mn and Ce and supported by SBA-15 was prepared by the “two-solvents” method aiming at the possible application in catalytic converters for abatement of alkanes in waste (exhaust) gases. The catalyst characterization was carried out by SAXS, N2-physisorption, XRD, TEM, XPS, EPR and H2-TPR methods. The catalysts’ performance was evaluated by tests on the combustion of methane, propane and butane. The reaction kinetics investigation showed that the reaction orders towards propane and oxygen were 0.7 and 0.1, respectively. The negative reaction order towards the water (−0.3) shows an inhibiting effect on the water molecules. Based on the data from the instrumental methods, catalytic experiments and mathematic modeling of the reaction kinetics, one may conclude that the Mars–van Krevelen type of mechanism is the most probable for the reaction of complete propane oxidation over single Mn and bi-component Mn-Ce catalysts. The fine dispersion of manganese and cerium oxide and their strong interaction inside the channels of the SBA-15 molecular sieve leads to the formation of difficult to reduce oxide phases and consequently, to lower catalytic activity compared to the mono-component manganese oxide catalyst. It was confirmed that the meso-structure was not modified during the catalytic reaction, thus it can prevent the agglomeration of the oxide particles.

Keywords

• SBA-15
• Mn-Ce oxides
• catalytic combustion
• methane
• propane
• butane oxidation