Operando XAFS Deciphering Dynamic Evolution of Heteronuclear Cu-Ni From Atomic Sites to Atomic Clusters for Enhanced...

Area of Science:

• Materials Science
• Electrochemistry
• Catalysis

Background:

• Understanding atomic-level active sites is crucial for catalysis.
• Dynamic transformations in multimetallic systems are challenging to study.

Purpose of the Study:

• Investigate potential-dependent atomic reconstruction in Cu-Ni sites.
• Elucidate the mechanism of electrocatalytic CO2 reduction (eCO2RR).

Main Methods:

• Operando X-ray spectroscopy and microscopy.
• Electrochemical measurements.
• Theoretical calculations.

Main Results:

• Observed in-plane atomic reconstruction of Cu-Ni dimers into Cu-Ni atomic clusters (ACs).
• Cu-rich evolution optimized CO2 intermediate adsorption and protonation.
• Tailored Cu5-Ni ACs enhanced eCO2RR kinetics, selectivity, and stability.

Conclusions:

• Demonstrated potential-dependent dynamic reconstruction of heteronuclear atomic sites.
• Provided insights into atomic-level mechanisms for eCO2RR.
• Highlighted the role of geometric and electronic structure tuning in catalysis.