Enhanced CO₂ Reactive Capture and Conversion Using Aminothiolate Ligand-Metal Interface.

Area of Science:

• Catalysis
• Materials Science
• Electrochemistry

Background:

• Metallic catalyst modification with organic ligands is key for electrocatalytic CO2 reduction.
• Lack of fundamental understanding of ligand-metal interfaces hinders catalyst design.
• Current designs often rely on trial-and-error approaches.

Purpose of the Study:

• To elucidate the mechanism of CO2 reduction to multicarbon products on aminothiolate-coated copper (Cu) catalysts.
• To understand how ligand properties influence CO2 activation and C-C coupling.
• To provide a scientific basis for designing efficient CO2 reduction catalysts.

Main Methods:

• Density functional theory (DFT) calculations for mechanistic studies.
• Experimental electrocatalysis using aminothiolate-coated Cu catalysts.
• Analysis of catalyst performance based on varying ligand and Cu facet properties.

Main Results:

• CO2 reduction performance is sensitive to alkyl chain length, ligand coverage, configuration, and Cu facet.
• The aminothiolate ligand-Cu interface enhances CO2 activation and lowers C-C coupling barriers.
• Experimental results show a 1.5-fold increase in multicarbon product selectivity and a 2-fold increase in partial current density.

Conclusions:

• Ligand-metal interface design is a promising strategy for CO2 capture and conversion.
• Understanding interfacial mechanisms is crucial for optimizing catalyst performance.
• Aminothiolate-coated Cu catalysts show enhanced activity and selectivity for multicarbon product formation.