3DOM Perovskite Enabled Interfacial Microenvironment Regulation With Accelerated Complete Reconstruction to...

Area of Science:

• Electrochemistry
• Materials Science
• Catalysis

Background:

• Electrochemical CO2 reduction (CO2RR) converts emissions to chemicals but faces challenges in activity, selectivity, and durability.
• Copper oxides are promising for C2+ electrosynthesis, but their performance depends on dynamic oxide reconstruction influenced by the microenvironment.

Purpose of the Study:

• To engineer the interfacial microenvironment of copper oxide catalysts for improved CO2RR performance.
• To investigate the role of electrode architecture in directing oxide reconstruction and enhancing catalytic activity.

Main Methods:

• Constructed a 3D ordered macroporous (3DOM) architecture from layered perovskite La2CuO4.
• Investigated catalyst performance in flow cells and membrane-electrode assemblies.
• Utilized experimental and theoretical analysis to identify active sites and reaction mechanisms.

Main Results:

• The 3DOM architecture facilitated complete reconstruction of La2CuO4 into nano-copper with abundant grain boundaries.
• Achieved a high C2+ partial current density of 585 mA cm-2 in a flow cell.
• Demonstrated stable operation for ~200 h at 600 mA cm-2 with high C2+ selectivity in a membrane-electrode assembly.
• Identified undercoordinated, strained Cu atoms at grain boundaries as key active sites for C2+ formation.

Conclusions:

• Electrode-architecture-driven microenvironment engineering is a viable strategy for optimizing CO2RR catalysts.
• The 3DOM-La2CuO4 catalyst significantly outperforms bulk counterparts and other Cu-oxide catalysts.
• This approach offers a general pathway for designing high-performance catalysts for CO2 reduction.