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

This article focuses on the theoretical investigation of silver-based single-atom alloy catalysts (SAACs) for the electrocatalytic reduction of carbon dioxide (CO₂) into C1 products using density functional theory (DFT) and the computational hydrogen electrode (CHE) model. The study evaluates various transition metal dopants substituting silver atoms on stepped Ag(211) surfaces, analyzing their electronic properties, adsorption energies of reaction intermediates, and tendencies toward competing reactions such as hydrogen evolution and OH poisoning. Results indicate that iridium (Ir) and rhodium (Rh) dopants show the most promise by favoring CO reduction over desorption, suppressing hydrogen evolution, and resisting OH poisoning, whereas fourth-period metals like iron (Fe), cobalt (Co), nickel (Ni), and copper (Cu) tend to promote CO desorption or hydrogen evolution and are less effective for further CO₂ reduction. These findings suggest that Ir- and Rh-doped Ag single-atom alloys could serve as effective electrocatalysts for CO₂ conversion beyond CO formation.