High-Entropy Metal Sulfide Promises High-Performance Carbon Dioxide Reduction

Area of Science:

• Materials Science
• Electrochemistry
• Catalysis

Background:

• Efficient carbon dioxide (CO2) conversion demands stable catalysts with high selectivity and reactivity.
• Developing advanced catalysts is crucial for sustainable chemical synthesis and carbon utilization.

Purpose of the Study:

• To design and evaluate a high-entropy metal sulfide (CuAgZnSnS4) as a catalyst for CO2 reduction.
• To investigate the synergistic effects within the high-entropy material for enhanced catalytic performance.

Main Methods:

• Synthesis and characterization of the high-entropy metal sulfide CuAgZnSnS4.
• Electrochemical testing of CO2 reduction performance across a wide potential window.
• In situ measurements and theoretical calculations to elucidate reaction mechanisms.

Main Results:

• CuAgZnSnS4 achieved excellent CO2 reduction performance with faradaic efficiency for carbon products ≥ 90% over a 600 mV potential range.
• The catalyst demonstrated superior single-product selectivity, evidenced by a high FEHCOOH/FECO ratio of 29.03 at -1.28 V vs RHE.
• Synergistic effects in CuAgZnSnS4 were found to regulate the electronic structure at Sn active sites, promoting *OCHO adsorption over *H.

Conclusions:

• The high-entropy metal sulfide CuAgZnSnS4 is a highly effective catalyst for CO2 electroreduction.
• Synergistic effects in high-entropy materials can be leveraged to control surface electronic structures and enhance catalytic selectivity.
• This work provides insights into designing efficient electrocatalysts for CO2 conversion, suppressing hydrogen evolution, and improving single-product selectivity.