Computational Discovery of New C─C Coupling Electrocatalysts for CO₂ Electroreduction

Area of Science:

• Materials Science
• Electrochemistry
• Catalysis

Background:

• Catalyst development is crucial for efficient low-temperature CO2 electroreduction, aiming for sustainable fuels and chemicals.
• While transition metals are widely studied, perovskite oxides offer unexplored potential due to their unique electronic structures.

Purpose of the Study:

• To systematically screen perovskite oxides for CO2 electroreduction stability and electrochemical performance.
• To identify novel active sites and mechanisms for CO2 electroreduction, particularly C-C coupling.

Main Methods:

• A data-driven approach was used to evaluate the stability of approximately 1500 ABO3 perovskites under CO2 electroreduction conditions.
• The ATaO3 family was selected for synthesis and electrochemical investigation, including computational reaction pathway analysis.

Main Results:

• 31 stable perovskite candidates were identified from the initial screening.
• Potassium tantalate (KTaO3) exhibited C-C coupling with a C2 Faradaic Efficiency of 10% at 100 mAcm-2.
• The size of the A-site element in ATaO3 was found to be critical for C-C coupling efficiency.

Conclusions:

• Perovskite oxides, specifically ATaO3, are promising for electrocatalytic C-C coupling in CO2 reduction.
• A CO*–*CHO coupling mechanism was identified as driving C2 production.
• This research provides new material design strategies for electrocatalytic C-C coupling beyond traditional copper-based catalysts.