Deactivation and Regeneration of Mo/ZSM-5 Catalysts for Methane Dehydroaromatization

Abstract

The methane dehydroaromatization (DHA) was studied over a series of impregnated Mo/ZSM-5 catalysts with different molybdenum contents (1-10 wt.%). It was shown that total methane conversion was decreased by 30% during 12 h of DHA reaction. The benzene formation rate was increased from 0.5 to 13.9 mol C6H6/(gMo·s) when the molybdenum content in the catalyst was lowered from 10 to 1 wt.%. The deactivated Mo/ZSM-5 catalysts were studied by a group of methods: N2 adsorption, XRD, TGDTA, HRTEM and XPS. The content and condensation degree (C/H ratio) of the carbonaceous deposits was found to increase with an increase of either of the following parameters: molybdenum content (1-10 wt.%), reaction temperature (720-780 °C), space velocity (405-1620 h-1), reaction time (0.5-20 h). The stability of Mo/ZSM-5 catalysts in reaction-regeneration cycles was better when the time on stream was shorter. The regeneration conditions of deactivated Mo/ZSM-5 catalysts providing their stable operation under multiple reaction-regeneration cycles have been selected.