The variability of CO2 hydrogenation reaction demands new potential strategies to regulate the fine structure of the catalysts for optimizing the reaction pathways. Herein, we report a dual-site strategy to boost the catalytic efficiency of CO2-to-methanol (MA) conversion. A new descriptor, τ, was initially established for screening the promising candidates with low-temperature activation capability of CO2, and sequentially a high-performance catalyst was fabricated centred with oxophilic Mo single atoms, who was further decorated with Pt nanoparticles. In CO2 hydrogenation, the obtained dual-site catalysts possess a remarkably-improved MA generation rate (0.27 mmol gcat.-1 h-1). For comparison, the singe-site Mo and Pt-based catalysts can only produce ethanol (EA) and formate acid (FA) at a relatively low reaction rate (0.11 mmol gcat.-1 h-1 for EA and 0.034 mmol gcat.-1 h-1 for FA), respectively. Mechanism studies indicate that the introduction of Pt species could create an active hydrogen-rich environment, leading to the alterations of the adsorption configuration and conversion pathways of the *OCH2 intermediates on Mo sites. As a result, the catalytic selectivity was successfully switched.
Keywords: CO2 hydrogenation; Dual-site catalyst; Oxophilicity; catalysis; selectivity.
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