Sequential *CO management via controlling in situ reconstruction for efficient industrial-current-density CO₂-to-C₂₊...

Area of Science:

• Electrochemistry
• Materials Science
• Catalysis

Background:

• Efficient carbon dioxide reduction (CO2R) to C2+ products requires precise control over *CO coverage and dimerization on copper (Cu) catalysts.
• Catalyst reconstruction during CO2R often leads to unpredictable surface changes, hindering rational design for high performance.

Purpose of the Study:

• To develop a method for constructing Cu arrays with controlled (100) facets for enhanced CO2R.
• To achieve sequential management of *CO coverage and dimerization for high selectivity and partial current density in CO2R.

Main Methods:

• Utilizing synchronous ligand leaching to guide the seeding-growth process during CO2R-induced catalyst reconstruction.
• Constructing Cu arrays with preferential (100) facets through controlled reconstruction.
• Investigating the effects of gradient diffusion on *CO coverage and dimerization kinetics.

Main Results:

• Successfully fabricated Cu arrays with dominant (100) facets via ligand-assisted reconstruction.
• Achieved high *CO coverage due to gradient diffusion, enabling high partial current density for C2+ products.
• Demonstrated enhanced C2+ selectivity attributed to lower *CO dimerization energy barriers on (100) facets.
• Attained an industrial-relevant Faradaic efficiency (FE) of 86.1% for C2+ and 60.8% for C2H4 at 700 mA cm-2.

Conclusions:

• Sequential *CO management on reconstructed Cu arrays with (100) facets is a viable strategy for high-performance CO2R.
• The developed method provides atomic-molecular scale insights into catalyst evolution and reaction intermediates, applicable to various electrocatalytic reactions.