Single-cluster anchored on PC₆ monolayer as high-performance electrocatalyst for carbon dioxide reduction reaction:...

Area of Science:

• Catalysis
• Materials Science
• Electrochemistry

Background:

• Carbon dioxide reduction reaction (CO2RR) faces challenges in catalyst activity and selectivity.
• Single-atom catalysts are limited by linear scaling relationships between intermediate adsorption energies.

Purpose of the Study:

• To investigate the CO2RR catalytic performance of triple metal clusters (M3@PC6) doped on a PC6 monolayer.
• To explore the potential of triple-atom anchored catalysts (TACs) for efficient CO2 conversion.

Main Methods:

• Density functional theory (DFT) calculations were employed.
• Investigated various triple metal clusters (M = Cr, Mn, Fe, Co, Ni, Cu, Pd, Rh) doped on PC6.

Main Results:

• Mn3@PC6, Fe3@PC6, and Co3@PC6 demonstrated high activity and selectivity for CO2 to CH4 reduction.
• Achieved limiting potentials of -0.32, -0.28, and -0.31 V, respectively.
• M3@PC6 catalysts exhibited enhanced regulation of intermediate binding strengths via charge and conformational self-adjustment.

Conclusions:

• PC6-based TACs show significant potential for CO2RR.
• The multi-center active sites in M3@PC6 overcome single-site limitations.
• This work provides guidance for applying TACs in broader electrochemical reactions.