Platinum and Frustrated Lewis Pairs on Ceria as Dual‐Active Sites for Efficient Reverse Water‐Gas Shift Reaction at Low Temperatures

Abstract

AbstractThe low‐temperature reverse water‐gas shift (RWGS) reaction faces the following obstacles: low activity and unsatisfactory selectivity. Herein, the dual‐active sites of platinum (Pt) clusters and frustrated Lewis pair (FLP) on porous CeO2 nanorods (Ptcluster/PN−CeO2) provide an interface‐independent pathway to boost high performance RWGS reaction at low temperatures. Mechanistic investigations illustrate that Pt clusters can effectively activate and dissociate H2. The FLP sites, instead of the metal and support interfaces, not only enhance the strong adsorption and activation of CO2, but also significantly weaken CO adsorption on FLP to facilitate CO release and suppress the CH4 formation. With the help of hydrogen spillover from Pt to PN−CeO2, the Ptcluster/PN−CeO2 catalysts achieved a CO yield of 29.6 %, which is very close to the thermodynamic equilibrium yield of CO (29.8 %) at 350 °C. Meanwhile, the Ptcluster/PN−CeO2 catalysts delivered a large turnover frequency of 8720 h−1. Moreover, Ptcluster/PN−CeO2 operated stably and continuously for at least 840 h. This finding provides a promising path toward optimizing the RWGS reaction.