Three-Component CO₂ Conversion to Carbonyl Carboxylates Catalyzed by a Copper-Based Metal-Organic Framework under...

Area of Science:

• Materials Science
• Catalysis
• Green Chemistry

Background:

• Sustainable carbon utilization is critical for mitigating climate change.
• Converting carbon dioxide (CO2) into valuable chemicals requires efficient catalytic systems.
• Existing methods often rely on noble-metal catalysts and harsh reaction conditions.

Purpose of the Study:

• To develop a novel, stable, and reusable catalyst for CO2 conversion.
• To investigate a new catalytic system for the three-component reaction of CO2 with alcohols.
• To achieve high yields of carbonyl carboxylates under mild conditions.

Main Methods:

• Synthesis of a novel copper-based metal-organic framework (Cu-MOF) with 1D channels.
• Characterization of the Cu-MOF's stability across a wide pH range and in various organic solvents.
• Catalytic testing of the Cu-MOF in the three-component reaction of CO2 with propargylic and monohydric alcohols.

Main Results:

• The synthesized Cu-MOF (1) exhibits high stability (pH 1-13) and solvent tolerance.
• Cu-MOF (1) efficiently catalyzes the CO2-involved three-component reaction, achieving >99% yield.
• The catalyst demonstrates broad substrate generality and recyclability for at least five cycles without significant activity loss.

Conclusions:

• This work presents the first 2D MOF capable of catalyzing the target CO2 transformation under mild conditions.
• The Cu-MOF offers a promising noble-metal-free catalytic system for sustainable CO2 conversion.
• Synergistic effects between Cu centers and the framework contribute to the catalytic efficiency.