Computational screening of silver-based single-atom alloys catalysts for CO2 reduction

Area of Science:

• Materials Science
• Electrochemistry
• Catalysis

Background:

• Electrocatalytic CO2 reduction to value-added products is crucial but challenging.
• Single-atom alloys (SAAs) offer enhanced catalytic properties for such reactions.

Purpose of the Study:

• To predict the efficacy of silver-based SAAs as electrocatalysts for CO2 conversion into C1 products.
• To investigate the influence of dopants on catalytic activity, selectivity, and stability.

Main Methods:

• Density functional theory (DFT) calculations.
• Computational electrode model using the Ag(211) surface.
• Assessment of surface defects, OH poisoning, and hydrogen evolution reaction (HER).

Main Results:

• Most dopants showed weak host-dopant mixing, affecting intermediate adsorption and reaction pathways.
• Copper-doped SAAs and other fourth-period metals favored CO desorption or HER.
• Iridium (Ir) and Rhodium (Rh) dopants promoted CO reduction over desorption and suppressed HER.

Conclusions:

• Silver-based SAAs with Ir and Rh dopants show significant potential for selective CO2 electroreduction.
• These dopants offer improved catalytic performance and stability against OH poisoning compared to other tested materials.