Boosting CO2 reduction catalyzed by tetragonal metal chalcogenides: a DFT study

Abstract

Converting carbon dioxide into higher-value fuels is one of the most promising strategies to overcome the dilemma caused by rising global energy demands and impending climate change. To examine the catalytic efficiency of the carbon dioxide reduction reaction (CRR), we performed a detailed investigation using density functional theory (DFT) calculations, focusing on tetragonal transition metal chalcogenides decorated with transition metal atoms. The results indicate that CH₄ is thermodynamically preferred via 8e⁻ reduction when CO₂ reduction is catalyzed by Co–FeS under the limiting potential of −0.41 V, and the underlying origin of its good activity stems from the strong adsorption of the *CHO intermediate. This research explores the application of tetragonal transition metal chalcogenides in energy conversion and storage and provides new insights for designing catalysts for CRR with good activity and selectivity.