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

Area of Science:

• Materials Science
• Electrochemistry
• Catalysis

Background:

• Rising global energy demands and climate change necessitate efficient carbon dioxide conversion into valuable fuels.
• Electrocatalytic reduction of carbon dioxide (CO2) is a key strategy for sustainable energy solutions.
• Transition metal chalcogenides offer potential as catalysts for CO2 reduction.

Purpose of the Study:

• To investigate the catalytic efficiency of tetragonal transition metal chalcogenides decorated with transition metal atoms for the carbon dioxide reduction reaction (CRR).
• To identify optimal catalyst materials and understand the reaction mechanisms for efficient CO2 conversion.

Main Methods:

• Density functional theory (DFT) calculations were employed to study various decorated transition metal chalcogenides.
• Calculations focused on determining thermodynamic preferences and limiting potentials for CO2 reduction pathways.
• Intermediate adsorption energies were analyzed to elucidate catalytic activity origins.

Main Results:

• Methane (CH4) was found to be the thermodynamically preferred product via an 8-electron reduction pathway.
• Cobalt-iron sulfide (Co-FeS) exhibited excellent catalytic activity for CO2 reduction, with a limiting potential of -0.41 V.
• The high activity of Co-FeS is attributed to the strong adsorption of the *CHO intermediate.

Conclusions:

• Tetragonal transition metal chalcogenides are promising materials for energy conversion and storage applications.
• The study provides insights into designing highly active and selective catalysts for the carbon dioxide reduction reaction.
• Co-FeS emerges as a potential catalyst for efficient methane production from CO2.