Self-adaptive Coordination Evolution Mediated Pore-Space-Partition in Metal-Organic Frameworks for Boosting SF₆/N₂...

Area of Science:

• Materials Science
• Chemistry
• Environmental Science

Background:

• Metal-organic frameworks (MOFs) are crucial for developing functional materials like porous adsorbents.
• Isoreticular chemistry enables precise structural control of MOFs for tailored applications.
• Efficient capture of greenhouse gases such as sulfur hexafluoride (SF₆) is an environmental priority.

Purpose of the Study:

• To construct novel pore space partitioned MOFs (CTGU-47-Mn/Fe) using a self-adaptive coordination evolution (SACE) strategy.
• To investigate the enhanced performance of these MOFs in SF₆ capture and recovery.
• To elucidate the mechanism behind the improved adsorption selectivity.

Main Methods:

• Synthesis of two pore space partitioned MOFs (CTGU-47-Mn/Fe) via SACE of polynuclear metal clusters.
• Gas adsorption and selectivity measurements using SF₆/N₂ mixtures.
• Theoretical calculations to understand SF₆-N₂ binding interactions.

Main Results:

• Successfully constructed CTGU-47-Mn/Fe MOFs with pore space partitioning (PSP).
• Achieved significantly enhanced SF₆ adsorption selectivity (from 37/72 to 634/157) compared to non-partitioned analogs (CTGU-46-Mn/Fe).
• Demonstrated strengthened binding affinity for SF₆ over N₂ due to PSP and F⋅⋅⋅H interactions.

Conclusions:

• The SACE strategy is effective for creating pore space partitioned MOFs.
• PSP in MOFs enhances SF₆ capture performance and selectivity.
• This work advances crystal engineering for developing superior porous adsorbents.