Breaking the Conversion-Selectivity\nTrade-Off in Methanol\nSynthesis from CO<sub>2</sub> Using Dual Intimate Oxide/Metal Interfaces

The selective hydrogenation of carbon\ndioxide (CO<sub>2</sub>)\nto value-added chemicals, e.g., methanol, using green hydrogen retrieved\nfrom renewable resources is a promising approach for CO<sub>2</sub> emission reduction and carbon resource utilization. However, this\nprocess suffers from the competing side reaction of reverse water–gas\nshift (RWGS) and methanol decomposition, which often leads to a strong\nconversion-selectivity trade-off and thus a poor methanol yield. Here,\nwe report that InO<sub><i>x</i></sub> coating of PdCu bimetallic\nnanoparticles (NPs) to construct intimate InO<sub><i>x</i></sub>/Cu and InO<sub><i>x</i></sub>/PdIn dual interfaces\nenables the break of conversion-selectivity trade-off by achieving\n∼80% methanol selectivity at ∼20% CO<sub>2</sub> conversion\nclose to the thermodynamic limit, far superior to that of conventional\nmetal catalysts with a single active metal/oxide interface. Comprehensive\nmicroscopic and spectroscopic characterization revealed that the InO<sub><i>x</i></sub>/PdIn interface favors the activation of\nCO<sub>2</sub> to formate, while the adjacent InO<sub><i>x</i></sub>/Cu interface readily converts formate intermediates to methoxy\nspecies in tandem, which thus cooperatively boosts methanol production.\nThese findings of dual-interface synergies via oxide coating of bimetallic\nNPs open a new avenue to the design of active and selective catalysts\nfor advanced catalysis.