Breaking scaling relations for efficient CO₂ electrochemical reduction through dual-atom catalysts

Area of Science:

• Catalysis
• Materials Science
• Electrochemistry

Background:

• Electrochemical reduction of carbon dioxide (CO2) is a promising strategy for energy crisis and carbon emission mitigation.
• Catalytic efficiency is often limited by scaling relations between intermediate adsorption energies.

Purpose of the Study:

• To design novel heteronuclear dual-atom catalysts to overcome scaling relation restrictions.
• To investigate the potential of these catalysts for efficient CO2 electroreduction to methane (CH4).

Main Methods:

• First-principles calculations were employed to screen 21 heteronuclear transition-metal dimers embedded in monolayer C2N.
• Free energy profiles were analyzed to determine catalytic activity and limiting potentials.

Main Results:

• The designed dual-atom catalysts decouple adsorption energies of key intermediates by assigning specific roles to each metal atom.
• CuCr/C2N and CuMn/C2N exhibited excellent performance for CO2 to CH4 reduction, with low limiting potentials of -0.37 V and -0.32 V, respectively.

Conclusions:

• Introducing multiple active sites in porous 2D materials can effectively break scaling relations.
• This approach offers a viable pathway for developing highly efficient electrocatalysts for multi-intermediate reactions like CO2 reduction.