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Solvent Exchange Dynamics in M2(dobdc): An Interplay among Binding Strength, Exchange Kinetics, and Cooperativity.
Hochul Woo1,2, John W Robinson1, Adam J Matzger1,2
1Department of Chemistry, University of Michigan, 930 North University Avenue, Ann Arbor, Michigan 48109, United States.
Journal of the American Chemical Society
|June 21, 2024
Summary
Metal-organic frameworks (MOFs) require careful solvent exchange for activation. This study reveals that solvent exchange rates depend on kinetic barriers and cooperativity, not just binding strength, offering insights for MOF activation protocols.
Area of Science:
- Materials Science
- Chemical Engineering
- Physical Chemistry
Background:
- Solvent exchange is critical for activating metal-organic frameworks (MOFs).
- Activation conditions vary significantly, even for similar MOFs.
- Understanding solvent exchange is key to optimizing MOF performance.
Purpose of the Study:
- To investigate factors influencing solvent exchange in isostructural M₂(dobdc) MOFs (M=Mg, Co, Zn).
- To differentiate early-stage exchange from the removal of residual solvents.
- To elucidate the relationship between solvent binding energy, exchange kinetics, and cooperativity.
Main Methods:
- Single-crystal Raman spectroscopy and bulk solvent phase analysis.
- Thermogravimetric analysis (TGA) and infrared (IR) spectroscopy.
- Density functional theory (DFT) calculations.
Main Results:
- Solvent exchange kinetics are influenced by cooperativity in both forward and reverse directions.
- Exchange rates are governed by kinetic barriers, not solely solvent binding affinity.
- Identified interplay between binding strength, kinetics, and cooperativity in MOF solvent exchange.
Conclusions:
- Solvent exchange rates in MOFs are complex, involving kinetic barriers and cooperative effects.
- Findings provide a deeper understanding of MOF activation processes.
- Offers guidance for developing efficient MOF activation protocols.
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