CO₂-Based Stable Porous Metal-Organic Frameworks for CO₂ Utilization.

Area of Science:

• Materials Science
• Chemical Engineering
• Environmental Science

Background:

• Carbon dioxide (CO2) transformation into functional materials is crucial for global sustainability.
• Metal-organic frameworks (MOFs) show promise for CO2 capture and conversion.
• Developing stable, porous MOFs directly from CO2 remains a significant challenge.

Purpose of the Study:

• To develop a facile method for synthesizing stable zirconium-based MOFs using CO2.
• To investigate the CO2 adsorption and catalytic conversion capabilities of these novel MOFs.
• To establish a dual CO2 utilization strategy through MOF synthesis and application.

Main Methods:

• Synthesis of zirconium-based MOFs (CO2-Zr-DEP and CO2-Zr-DEDP) via sequential desilylation-carboxylation-coordination.
• Characterization using powder X-ray diffraction and high-resolution transmission electron microscopy.
• Incorporation of Ag(I) to form a heterogeneous catalyst for CO2 conversion.

Main Results:

• Stable zirconium-based MOFs with face-centered cubic topology were successfully synthesized using CO2.
• The MOFs exhibited high surface area (up to 3688 m2 g-1) and CO2 adsorption capacity (up to 12.5 wt %).
• The Ag(I)-integrated MOF catalyst efficiently converted CO2 and propargylic alcohols into cyclic carbonates (>99% yield at room temperature).

Conclusions:

• A novel, facile methodology for CO2-based MOF synthesis was established.
• The synthesized MOFs offer a dual approach for CO2 utilization via capture and catalytic conversion.
• This work significantly advances strategies for enhanced overall CO2 utilization.