The empirical optimization of the preparation of catalytically active copper-containing catalysts is far more advanced than the fundamental understanding of the catalyst performance because of the structural complexity of the catalysts. Here, we demonstrate the interplay between the catalyst structure and CO 2 hydrogenation on Cu catalysts boosted with nickel species. The nickel dispersion on copper markedly affects the CO 2 dissociation activity and catalytic reaction pathways, thus resulting in distinctive catalytic activity and selectivity attributed to Ni. Specifically, the catalyst incorporating nickel alloyed in copper maximizes the synergy between the two metals and is characterized by conversions close to the thermodynamic equilibrium to CO as a productwith switched off methanationover a wide temperature range. Catalyst performance data, spectra characterizing the catalyst, and theoretical results demonstrate that surface copper with adjacent nickel atoms efficiently activates CO 2 via a redox mechanismwith adsorption of CO being suppressedso that methanation associated with deep hydrogenation of CO is inhibited. The results of this investigation highlight the importance of structures with copper-adjacent-nickel, which appear to offer appealing opportunities for tailoring efficient copper-containing catalysts for CO 2 hydrogenation.

Conversion of CO2 into chemicals is a promising way for CO2 utilization, but its intricate transformation pathways and insufficient product selectivity are still challenging. Exploiting new catalysts for tuning product...

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