Constructing Asymmetric Cu Catalytic Sites for CO₂ Electroreduction with Higher Selectivity to C₂ Products

Area of Science:

• Catalysis
• Materials Science
• Electrochemistry

Background:

• Developing efficient catalysts for CO2 reduction is crucial for carbon neutrality and producing valuable chemicals.
• Precisely controlling catalytic sites to direct CO2 reduction products remains a significant challenge.
• Metal-organic frameworks (MOFs) offer tunable platforms for designing advanced catalytic materials.

Purpose of the Study:

• To investigate how different coordination environments in MOF-derived catalysts affect electrochemical CO2 reduction reaction (eCO2RR) performance.
• To understand the relationship between catalyst structure and selectivity towards specific CO2 reduction products.
• To provide insights for designing more effective catalysts for CO2 utilization.

Main Methods:

• Synthesized MOF-derived catalysts with distinct coordination environments (Cu-N2O2 and Cu-N2O3).
• Evaluated catalyst performance using electrochemical CO2 reduction reactions.
• Analyzed catalyst structures to correlate coordination environment with catalytic activity and selectivity.

Main Results:

• Cu-N2O2-derived catalysts, featuring asymmetric Cu0 and Cu+ sites, showed higher selectivity for C2 products compared to Cu-N2O3 catalysts.
• Cu-N2O3 catalysts exhibited only symmetric Cu0 sites.
• The synergistic interaction between Cu0 and Cu+ sites in Cu-N2O2 catalysts facilitated multi-electron transfer and enhanced CO2 activation.

Conclusions:

• The coordination environment of MOF-derived catalysts significantly impacts their selectivity in eCO2RR.
• Asymmetric catalytic centers (Cu0/Cu+) are more effective for promoting C2 product formation than symmetric centers (Cu0).
• This study offers valuable guidance for designing tailored MOF-based catalysts for efficient CO2 conversion.