Unexpected high selectivity for acetate formation from CO2 reduction with copper based 2D hybrid catalysts at ultralow potentials

Copper-based catalysts are efficient for CO2 reduction affording commodity chemicals. However, Cu(i) active species are easily reduced to Cu(0) during the CO2RR, leading to a rapid decay of catalytic performance. Herein, we report a hybrid-catalyst that firmly anchors 2D-Cu metallic dots on F-doped CuxO nanoplates (CuxOF), synthesized by electrochemical-transformation under the same conditions as the targeted CO2RR. The as-prepared Cu/CuxOF hybrid showed unusual catalytic activity towards the CO2RR for CH3COO- generation, with a high FE of 27% at extremely low potentials. The combined experimental and theoretical results show that nanoscale hybridization engenders an effective s,p-d coupling in Cu/CuxOF, raising the d-band center of Cu and thus enhancing electroactivity and selectivity for the acetate formation. This work highlights the use of electronic interactions to bias a hybrid catalyst towards a particular pathway, which is critical for tuning the activity and selectivity of copper-based catalysts for the CO2RR.

Automated summary

The study presents a hybrid catalyst synthesized through electrochemical transformation, which can effectively enhance the activity and selectivity of copper-based catalysts in the CO2 reduction reaction. By anchoring 2D-Cu metallic dots on F-doped CuxO nanoplates, the hybrid catalyst achieved high efficiency in generating CH3COO- at extremely low potentials.