Development of Ti-modified Cr/MCM-41 catalysts for oxidative dehydrogenation of isobutane
摘要
This study aimed to synthesize Cr-based catalysts with high activity, selectivity, and hydrothermal stability for oxidative dehydrogenation (ODH) of isobutane. Firstly, the thermodynamic equilibrium calculations were carried out to estimate the equilibrium conversions of isobutane at various i-C4H10/CO2 molar ratios. Equilibrium calculations were shown the suitability of reaction studies at 600 °C. Then, a series of Ti-modified xCr/Ti-MCM-41 was prepared using the hydrothermal synthesis method with Cr loadings of 3 and 10 wt%, while Ti content was kept constant at 2.5wt.%. The effects of Cr loading and feed composition on catalytic performance were also investigated in a fixed bed reactor. The optimal i-C4H10/CO2 molar feed ratio was found to be 1/5. The catalysts containing 10 wt% Cr exhibited the highest isobutane conversion(~ 90%) and isobutene selectivity(~ 85%). It was discussed that the enhanced hydrophilic properties provided by the Ti-modification contributed to high conversion and selectivity. The effect of reactor temperature on activity was investigated at 500 °C and 600 °C (WHSV: 51 h− 1). Reverse water gas shift reaction (RWGS) did not occur at lower temperatures, resulting in lower isobutane conversion and isobutene selectivity values. The reaction was also performed at two different WHSVs(51 h− 1 and 72 h− 1). At higher WHSV, which corresponds to shorter contact times, lower isobutene selectivity values were observed, due to the difficulty of reactant adsorption on the catalyst surface. It was also noted that at shorter contact times, the RWGS reaction did not occur initially, and the presence of excess CO2 increased surface acidity.