Low-Coordination Triangular Cu₃ Motif Steers CO₂ Photoreduction to Ethanol

Area of Science:

• Catalysis
• Materials Science
• Renewable Energy

Background:

• Photoreduction of carbon dioxide (CO2) to C2+ products using copper-based multi-atom catalysts (MACs) is promising.
• Challenges include low metal content, competing ethylene production, and poor ethanol yield.

Purpose of the Study:

• To develop an ultra-high-density copper MAC for efficient ethanol production from CO2.
• To investigate the catalytic mechanism and structure-activity relationship.

Main Methods:

• A "pre-locking and nanoconfined polymerization" strategy was employed to synthesize Cu3 MACs.
• Characterization of the catalyst's structure, composition, and electronic properties.
• Evaluation of catalytic performance for CO2 photoreduction under simulated sunlight.

Main Results:

• Synthesized an ultra-high-density Cu MAC (36 wt% Cu) with low-coordination triangular Cu3 motifs.
• Achieved high reactivity (117 µmol g-1 h-1) and selectivity (98%) for ethanol production.
• Identified coexisting Cu(I) and Cu(II) in Cu3 motifs as key to CO2 activation and C-C coupling.

Conclusions:

• The developed Cu3 MAC demonstrates superior performance for CO2 photoreduction to ethanol.
• The triangular Cu3 configuration facilitates CO2 adsorption, electron accumulation, and preferential ethanol formation.
• This work offers a new strategy for designing high-performance MACs for sustainable chemical production.