Abstract

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.

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