Dynamic Proton Extraction from Supramolecular Functionalized Metal-Organic Framework/Ti₃C₂ MXene Hybrids for...

Area of Science:

• Materials Science
• Catalysis
• Photochemistry

Background:

• Nitrogen (N₂) photoreduction to ammonia (NH₃) requires efficient proton supply and N₂ activation via photogenerated holes and electrons.
• Optimizing charge carrier generation and catalytic sites is key for high N₂-to-NH₃ conversion efficiency.

Purpose of the Study:

• To design a robust photothermal catalyst for efficient N₂ photoreduction.
• To investigate the synergistic effects of MIL-125(Ti), perylene tetracarboxylic acid (PTA), and MXene for solar ammonia synthesis.

Main Methods:

• Fabrication of a carboxyl-enriched supramolecular (PTA) functionalized MIL-125(Ti)/MXene catalyst.
• Characterization of the catalyst's structure-activity relationship and photothermal properties.
• Evaluation of solar-to-ammonia conversion rates under varying illumination intensities.

Main Results:

• The designed catalyst exhibits synergistic collaboration between MIL-125(Ti) for N₂ activation, PTA for proton supply, and MXene for photothermal response.
• Enhanced light harvesting and responsiveness facilitate dynamic multielectron/proton extraction.
• Remarkably high solar-to-ammonia conversion rates of 314.5–654.7 μmol g⁻¹ h⁻¹ were achieved.

Conclusions:

• The developed photothermal catalyst enables efficient solar-driven ammonia production.
• The study provides insights into rational catalyst design for solar ammonia synthesis systems.
• This work highlights the potential of functionalized MIL-125(Ti)/MXene composites in sustainable ammonia production.