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

Wenbin Li, Jie Gan, Yuxuan Liu, Yong Zou, Sai Zhang, Yongquan Qu

2023Angewandte Chemie International Edition113 citationsDOIOpen Access PDF

Abstract

Abstract The 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 CeO 2 nanorods (Pt cluster /PN−CeO 2 ) 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 H 2 . The FLP sites, instead of the metal and support interfaces, not only enhance the strong adsorption and activation of CO 2 , but also significantly weaken CO adsorption on FLP to facilitate CO release and suppress the CH 4 formation. With the help of hydrogen spillover from Pt to PN−CeO 2 , the Pt cluster /PN−CeO 2 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 Pt cluster /PN−CeO 2 catalysts delivered a large turnover frequency of 8720 h −1 . Moreover, Pt cluster /PN−CeO 2 operated stably and continuously for at least 840 h. This finding provides a promising path toward optimizing the RWGS reaction.

Topics & Concepts

NanorodCatalysisWater-gas shift reactionFrustrated Lewis pairChemistryYield (engineering)AdsorptionPlatinumChemical engineeringMaterials scienceLewis acids and basesNanotechnologyPhysical chemistryOrganic chemistryMetallurgyEngineeringCatalytic Processes in Materials ScienceMetal-Organic Frameworks: Synthesis and ApplicationsAdvanced Photocatalysis Techniques