AbstractThe oxidative dehydrogenation of propane using CO2 (CO2‐ODH) technology has broad application prospects in the production of propylene and the utilization of CO2, and the development of efficient CO2‐ODH catalysts is of great significance. However, it remains a challenge to develop a highly efficient catalyst that can activate both C─H and C═O. Herein, a PtZn/Co@S‐1 catalyst with a very low precious metal content of 0.2 wt.% is reported. Benefiting from the PtZn4 nanoclusters dispersed on the surface of Silicalite‐1 zeolite and tetrahedrally coordinated Co2+ in the Silicalite‐1 zeolite framework via relay catalysis, the independent dual sites structure (PtZn/Co@S‐1) greatly promotes CO2‐ODH reaction with a high conversion rate of both C3H8 (59.7%) and CO2 (44.3%), and propylene selectivity of 94.9%, thus upsetting the equilibrium for direct dehydrogenation of propane. Experimental measurements and density functional theory calculations suggest that the PtZn4 and Co2+ interfaces are likely propane dehydrogenation and carbon dioxide hydrogenation active sites respectively.
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