Highly dispersed atomic layer deposited CrOx on SiO2 catalyst with enhanced yield of propylene for CO2 –mediated oxidative dehydrogenation of propane

Abstract

The increasing worldwide demand for propylene and the necessity of CO2 mitigation attracted the attention of scientists to focus on CO2-oxidative dehydrogenation of propane (CO2-ODHP). In this regard, CrOx/SiO2 catalyst is an important and conventional option. Herein, we studied the atomic layer deposition (ALD) of CrOx on silica to increase the propylene production by increasing the dispersion of the catalyst. For ALD synthesis of CrOx/SiO2 catalyst, Cr(acac)3 and synthetic air were used as metal precursor and oxidant. The catalysts were examined in the CO2-ODHP reaction and their characteristics were compared to their impregnation counterparts using UV–Vis DRS, Raman, XANES, HRTEM and STEM-EDS mapping, H2-TPR, NH3-TPD and TPO. The ALD catalysts have shown up to 2 times higher acidity and enhanced reducibility compared to the impregnation catalysts. The presence of mainly Cr(VI) with a pre-edge peak at 5.994 keV in both series of catalysts was confirmed by XANES. UV–Vis DRS and Raman spectroscopy revealed the higher contents of active polymeric Cr(VI) species in the ALD ones. The dark field HRTEM and STEM-EDS mapping represented higher dispersion of chromium oxide particles in ALD catalysts. In CO2-ODHP, the ALD catalysts showed up to 18 and 15% promotion in propane conversion and propylene yield.