A DFT Study on the Selective Oxidation of Ethane Over Pure SBA-15 and SBA-15-supported Vanadium Oxide

Abstract

The selective oxidation of ethane over pure SBA-15 and V/SBA-15 were theoretically studied by density functional theory. The cluster models of pure SBA-15 and V/SBA-15 were proposed. The structure properties of these two models were calculated and were found to be in good agreement with experimental values. The catalytic reaction pathways for the ethane oxidation to acetaldehyde and ethylene were determined. Our results show that the hydroxyl groups on pure SBA-15 can activate the gas-phase O₂ to form a peroxide species, which acts as the active site for the selective oxidation of ethane. The formation of ethylene is much more preferred than that of acetaldehyde over pure SBA-15. For V/SBA-15, the peroxide species also acts as the active center. The energy barrier of C–H bond activation over V/SBA-15 is by 14.63 kJ/mol lower than that over pure SBA-15. The formation of acetaldehyde is preferred than that of ethylene over V/SBA-15. On the basis of our results, the reaction mechanisms of ethane selective oxidation over pure SBA-15 and V/SBA-15 were systematically compared and discussed. The theoretical results in this study are in good agreement with our previous experimental results. They can reasonably explain the catalytic nature of pure SBA-15 and the effect of vanadium, opening new perspectives in the understanding of the chemistry of SBA-15.