The increase in global demand for propylene coupled with the deficiencies in the co-production of propylene from steam crackers necessitated the development of on-purpose propylene production technologies. Similarly, the valorization of anthropogenic CO2 can contribute in the reduction of GHGs emissions. The oxidative dehydrogenation of propane (ODH-CO2) using CO2 as a mild oxidant can potentially serve the aforementioned purposes. The role of CO2 in the oxidative dehydrogenation (ODH) includes the reverse water-gas shift reaction, active sites regeneration through restoration of reactive oxygen species, reducing site deactivation by suppressing coke formation and blocking unselective electrophilic oxygen species. In this work, the reaction was investigated over monometallic and bimetallic GaV oxide supported on modified ZSM-5 zeolite. Different morphologies of ZSM-5 (Si/Al = 280) including nanosize and large crystals, and different core-shell composites (ZS@MS and ZS@MSA) were prepared using hydrothermal and facile ammonia catalyzed sol-gel syntheses, respectively. The catalysts were synthesized using co-impregnation technique, and their crystal structures, active species dispersion and metal-support interactions were confirmed using XRD, BET, SEM/TEM, NH3/CO2 TPD, H2-TPR and TG/DTG techniques. The novelty of this work is in the various zeolite modification strategies leading to suitable interactions (metal-support) and enhanced dispersion of the active species, resulting in promising catalytic performance. Typically, GaOx-VOx over ZSM-5 nanosize catalyst exhibited 51.2 % C3= selectivity and 53 % conversion at 600 oC. The relationship between the interaction of active species with the modified zeolites and the catalytic performance is highlighted, and the stability of the catalysts coupled with their deactivation mechanisms in CO2-ODHP reaction is discussed.

CO2-assisted oxidative dehydrogenation of propane over bimetallic GaOx and VOx oxides supported on modified zeolites

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