Iron-Based Metal-Organic Frameworks as Platform for H₂S Selective Conversion: Structure-Dependent Desulfurization...

Area of Science:

• Materials Science
• Catalysis
• Chemical Engineering

Background:

• Selective conversion of hydrogen sulfide (H₂S) to sulfur is crucial for industrial processes.
• Metal-Organic Frameworks (MOFs) offer tunable platforms for catalytic applications.

Purpose of the Study:

• Investigate structure-activity relationships in Fe-MOFs for H₂S to sulfur conversion.
• Elucidate the catalytic mechanism and identify key factors influencing performance.
• Develop rational design principles for efficient desulfurization catalysts.

Main Methods:

• Synthesis of three classical Fe-MOFs: MIL-100(Fe), MIL-101(Fe), and MIL-53(Fe).
• Physicochemical characterization using various techniques.
• Catalytic testing for H₂S selective conversion.
• Density Functional Theory (DFT) calculations.

Main Results:

• Fe-MOFs exhibited varying desulfurization performances based on their microstructures.
• MIL-100(Fe) showed the highest catalytic activity (100% H₂S conversion, 100% S selectivity at 100-180 °C), surpassing commercial Fe₂O₃.
• Performance differences correlate with the varying amounts of Lewis acid sites.

Conclusions:

• The number of Lewis acid sites is the primary factor determining the catalytic efficiency of Fe-MOFs for H₂S desulfurization.
• A catalytic mechanism for selective H₂S conversion over Fe-MOFs was proposed.
• This research provides insights for designing advanced desulfurization catalysts.