초록 |
The electrochemical conversion of CO2 into high-value C2+ chemicals using a renewable energy is a promising strategy for realizing carbon-neutral cycles, while high energetic barrier of C-C coupling reactions limits the product selectivity. Here, we propose that the close coupling of Cu with ceria at the nanometer level creates the synergistic interface for selective C-C coupling, and the Cu/ceria catalyst is demonstrated to achieve the selectivity values of 81.2% and 71.6% for the CO2 reduction reaction and C2+ production, respectively. The relative amount of Cu to Ce controls the density of the interfaces and Cu-Cu diatom sites, thus determining the selectivity of C2+ chemicals. The synergistic interface is proposed to weaken the hydrogen binding energy by the modification of electronic structure as well as strengthen C-C bond of the OCCO intermediate by the binding mode change, significantly lowering the reaction energy of the C-C coupling step with a broken scaling relation. This work offers new insights into the role of the metal-oxide interface in the electrochemical reduction of CO2 to high-value chemicals. |