Single-Atom Catalysts Supported on the Graphene/Graphdiyne Heterostructure for Effective CO₂ Electroreduction

Area of Science:

• Materials Science
• Electrochemistry
• Computational Chemistry

Background:

• Electrochemical reduction of carbon dioxide (CO2) to valuable chemicals is crucial for sustainable energy.
• Developing high-performance electrocatalysts for CO2 reduction reaction (CO2RR) is a significant challenge.

Purpose of the Study:

• To investigate transition metal (TM) anchored on nitrogen-doped graphene/graphdiyne heterostructures (TM-N4@GRA/GDY) as single-atom catalysts for CO2 electroreduction.
• To evaluate the catalytic activity and understand the underlying electronic structure for CO2RR.

Main Methods:

• Density functional theory (DFT) calculations were employed.
• Systematic investigation of TM-N4@GRA/GDY structures for CO2 electroreduction.
• Analysis of electronic structure and reaction mechanisms.

Main Results:

• Co-N4@GRA/GDY demonstrated excellent activity for CO2 to methane (CH4) conversion with a low limiting potential of -0.567 V.
• The reaction barrier was reduced to 0.366 eV in a continuum solvent due to enhanced electron transfer.
• The GRA/GDY heterostructure weakened the scaling relationship of intermediates, boosting catalytic activity compared to single graphene.

Conclusions:

• Co-N4@GRA/GDY is a promising single-atom catalyst for efficient electrochemical CO2 reduction.
• The GRA/GDY heterostructure design enhances catalytic performance by optimizing electronic interactions.
• This study offers insights for designing advanced electrocatalysts for CO2 utilization.