Non-Oxidative Propane Dehydrogenation on CrO x -ZrO 2 -SiO 2 Catalyst Prepared by One-Pot Template-Assisted Method.
Elena V GolubinaIgor Yu KaplinAnastasia V GorodnovaEkaterina S LoktevaOksana Ya IsaikinaKonstantin Igorevich MaslakovPublished in: Molecules (Basel, Switzerland) (2022)
A series of CrO x -ZrO 2 -SiO 2 (CrZrSi) catalysts was prepared by a "one-pot" template-assisted evaporation-induced self-assembly process. The chromium content varied from 4 to 9 wt.% assuming Cr 2 O 3 stoichiometry. The catalysts were characterized by XRD, SEM-EDX, temperature-programmed reduction (TPR-H 2 ), Raman spectroscopy, and X-ray photoelectron spectroscopy. The catalysts were tested in non-oxidative propane dehydrogenation at 500-600 °C. The evolution of active sites under the reaction conditions was investigated by reductive treatment of the catalysts with H 2 . The catalyst with the lowest Cr loading initially contained amorphous Cr 3+ and dispersed Cr 6+ species. The latter reduced under reaction conditions forming Cr 3+ oxide species with low activity in propane dehydrogenation. The catalysts with higher Cr loadings initially contained highly dispersed Cr 3+ species stable under the reaction conditions and responsible for high catalyst activity. Silica acted both as a textural promoter that increased the specific surface area of the catalysts and as a stabilizer that inhibited crystallization of Cr 2 O 3 and ZrO 2 and provided the formation of coordinatively unsaturated Zr 4+ centers. The optimal combination of Cr 3+ species and coordinatively unsaturated Zr 4+ centers was achieved in the catalyst with the highest Cr loading. This catalyst showed the highest efficiency.