Modulating the Asymmetric Atomic Interface of Copper Single Atoms for Efficient CO₂ Electroreduction.

Area of Science:

• Materials Science
• Electrochemistry
• Catalysis

Background:

• Copper single-atom catalysts (Cu SACs) show promise for electrocatalytic CO2 reduction reactions (ECRRs).
• Limited research exists on Cu SACs utilizing asymmetric atomic interfaces for efficient CO production.

Purpose of the Study:

• To design and investigate Cu SACs with distinct asymmetric atomic interfaces.
• To explore the impact of these interfaces on ECRR performance, particularly CO selectivity and activity.

Main Methods:

• Rational design of two Cu SACs: CuN3O/C and CuCO3/C.
• Electrochemical evaluation of catalytic performance, including Faradaic efficiency (FE) and turnover frequency (TOF).
• Density Functional Theory (DFT) calculations to elucidate reaction mechanisms.

Main Results:

• CuN3O/C achieved high ECRR selectivity (FE_CO > 90%) over a wide potential window (-0.5 to -0.9 V vs RHE), reaching 96% at -0.8 V.
• CuN3O/C exhibited a significantly higher TOF (up to 2782.6 h⁻¹) compared to CuCO3/C (max 4.8 h⁻¹).
• DFT results indicated a lower Gibbs free energy for CO desorption at the CuN3O site, explaining its superior performance.

Conclusions:

• Regulating asymmetric atomic interfaces by adjusting coordination atoms is an effective strategy to enhance ECRR selectivity and activity.
• The CuN3O/C catalyst demonstrates outstanding performance for ECRR to CO production.
• This study provides insights into designing advanced SACs for efficient CO2 conversion.