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Design of Pore-Space-Partitioned Metal-Organic Frameworks Using Spiro Ligand Chemistry.

Pooja Ajayan1, Wei Wang1, Ziyang Jia1

  • 1Department of Chemistry, University of California, Riverside, Riverside, California 92521, United States.

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|August 25, 2025
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Summary

Researchers developed novel metal-organic frameworks (MOFs) using spiro ligands for gas separation. These materials show high gas uptake and selective separation of industrially relevant gas mixtures.

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Area of Science:

  • Materials Science
  • Chemistry
  • Chemical Engineering

Background:

  • The design of crystalline porous materials often utilizes bioisosteric replacement strategies, replacing benzene rings with aliphatic cores.
  • Maintaining isoreticular chemistry during bioisosteric replacement, especially with flexible spiro ligands, presents significant challenges in metal-organic framework (MOF) design.
  • Few studies have explored spiro ligands for MOFs in gas separation applications due to their flexibility and deviation from para-benzene-based ligands.

Purpose of the Study:

  • To investigate the use of spiro ligands in designing isoreticular metal-organic frameworks (MOFs) for gas separation applications.
  • To demonstrate a pore-space-partition strategy for controlling ligand positioning and alignment in spiro-based MOFs.
  • To evaluate the gas sorption and separation performance of these novel MOFs.

Main Methods:

  • Employed a pore-space-partition strategy to create a multimodule system for spiro ligand assembly.
  • Synthesized a family of isoreticular MOFs using spiro[3.3]heptane-2,6-dicarboxylic acid and various tripyridyl-based pore-partition modules.
  • Investigated both homometallic (Fe) and heterometallic (CoV, CoFe) compositions.
  • Characterized gas sorption properties and evaluated gas mixture separation performance.

Main Results:

  • Successfully generated a family of isoreticular MOFs with a partitioned acs (pacs) structure using spiro ligands.
  • Achieved excellent sorption capacities for CO2 (61.9 cm3/g) and small hydrocarbons like C2H2 (116.3 cm3/g) and C2H4 (101.4 cm3/g).
  • Demonstrated inverse C2H6/C2H4 selectivity and promising separation performance for C2H2/CO2 (selectivity up to 5.5), C3H8/CH4 (selectivity up to 279), and C2H6/CH4 (selectivity up to 22.7).

Conclusions:

  • The pore-space-partition strategy enables precise control over spiro ligand assembly in MOFs, facilitating isoreticular chemistry.
  • The developed spiro-based MOFs exhibit superior gas sorption and selective separation capabilities, particularly for challenging gas mixtures.
  • This work expands the scope of MOF design using aliphatic bioisosteres for advanced gas separation technologies.