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Pore Environment Engineering in Al-MOFs Enables Thermodynamic-Kinetic Synergy for High-Resolution Chromatographic

Cheng-Yu Rong1, Shurui Gao1, Xiao-Yi Fu1

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Ligand functionalization of aluminum-based metal-organic frameworks (Al-MOFs) optimizes aromatic isomer separation. This strategy balances thermodynamics and kinetics, enhancing chromatographic performance for challenging separations.

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Area of Science:

  • Materials Science
  • Separation Science
  • Nanotechnology

Background:

  • Aluminum-based metal-organic frameworks (Al-MOFs) show potential for chromatographic separations.
  • Optimizing the thermodynamic-kinetic balance is crucial for separating aromatic isomers.
  • Existing Al-MOFs face challenges in achieving high-performance separation of closely related compounds.

Purpose of the Study:

  • To develop a ligand functionalization strategy for tuning the pore environment and separation performance of Al-MOFs.
  • To investigate the impact of alkoxy group introduction on the host-guest interactions and diffusion dynamics within Al-MOFs.
  • To achieve an optimal thermodynamic-kinetic balance for enhanced chromatographic separation of aromatic isomers.

Main Methods:

  • Synthesis of three isostructural Al-MOFs (Al-L-H, Al-L-OMe, Al-L-OCp) via ligand functionalization with methoxy (OMe) and cyclopentyloxy (OCp) groups.
  • Characterization of the synthesized materials to analyze pore structure and host-guest interactions.
  • Mechanistic studies to evaluate adsorption strength and molecular diffusion properties.

Main Results:

  • Alkoxy side chain introduction reduced porosity and modulated host-guest interactions in Al-MOFs.
  • Methoxy (OMe) substitution effectively weakened adsorption strength and enhanced molecular diffusion.
  • Al-L-OMe demonstrated superior separation efficiency, achieving a resolution of 13.74 for p-xylene and o-xylene.

Conclusions:

  • Ligand design and pore environment engineering are effective strategies for harmonizing thermodynamic and kinetic effects in Al-MOFs.
  • The developed Al-L-OMe material surpasses many reported MOF-based stationary phases for aromatic isomer separation.
  • This study offers a pathway toward high-performance chromatographic stationary phases through rational MOF design.