The selective hydrogenation of carbon dioxide (CO) to value-added chemicals, e.g., methanol, using green hydrogen retrieved from renewable resources is a promising approach for CO emission reduction and carbon resource utilization. However, this process suffers from the competing side reaction of reverse water-gas shift (RWGS) and methanol decomposition, which often leads to a strong conversion-selectivity trade-off and thus a poor methanol yield. Here, we report that InO coating of PdCu bimetallic nanoparticles (NPs) to construct intimate InO/Cu and InO/PdIn dual interfaces enables the break of conversion-selectivity trade-off by achieving ∼80% methanol selectivity at ∼20% CO conversion close to the thermodynamic limit, far superior to that of conventional metal catalysts with a single active metal/oxide interface. Comprehensive microscopic and spectroscopic characterization revealed that the InO/PdIn interface favors the activation of CO to formate, while the adjacent InO/Cu interface readily converts formate intermediates to methoxy species in tandem, which thus cooperatively boosts methanol production. These findings of dual-interface synergies via oxide coating of bimetallic NPs open a new avenue to the design of active and selective catalysts for advanced catalysis.
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http://dx.doi.org/10.1021/jacs.4c09106 | DOI Listing |
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