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[SOM-MIL-88A] Approach for High-Yield Synthesis of Single-Crystalline Ordered Macro-Microporous MOFs
Summary:
The authors from Tsinghua University developed a universal approach for synthesizing single-crystalline ordered macro-microporous metal-organic frameworks (SOM-MOFs), achieving high yields and enhanced stability in both water and acidic solutions.
Background:
1. Metal-organic frameworks (MOFs) have attracted significant attention due to their diverse applications in gas detection, biosensing, and catalysis. However, the development of single-crystalline ordered macro-microporous MOFs (SOM-MOFs) has been hindered by challenges in precursor stabilization and crystallization modulation. Previous methods resulted in low yields and limited stability profiles.
2. The authors proposed an innovative method using nonprotonic polar solvents to stabilize the precursor solution and modulate crystallization, resulting in the successful synthesis of SOM-MIL-88A with exceptional stability and performance.
Research Content:
1. Synthesis:
The authors synthesized SOM-MIL-88A using a dual-solvent system of dimethyl sulfoxide (DMSO) and ethanol. This method stabilized the precursor solution and modulated the crystallization process.
2. Characterizations:
1) BET surface area of SOM-MIL-88A was measured to be 49.88 m²/g, with a micropore volume of 0.57 cm³/g.
2) SEM and TEM tests showed a spindle-like morphology with well-defined 3D-ordered macroporous structures, particle sizes of approximately 240 nm, and uniform distribution of elements (C, O, Fe).
3) PXRD patterns confirmed the single-crystalline nature of SOM-MIL-88A.
3. Application:
SOM-MIL-88A demonstrated significant improvements in various applications:
- 2.67-fold higher adsorption efficiency for Kaumas Brilliant Blue R250 compared to MIL-88A.
- Higher yield (40.96%) and selectivity (67.36%) in the selective oxidation of benzyl alcohol to benzaldehyde.
- Enhanced enzyme loading (121 mg/g) and specific activity (833 U/mg) for lipase ET 2.0 immobilization.
- Superior performance in glucose conversion to hydroxyl radicals, with a linear detection range of 0.75–500 μM and a detection limit of 0.7 μM.
4. Mechanism:
DFT simulations revealed that DMSO reduced the surface energy of SOM-MIL-88A from 0.87 J/m² to 0.57 J/m², inhibiting Ostwald ripening and promoting oriented attachment. This balance resulted in the desired SOM morphology.
Outlook:
This research marks a significant advancement in the synthesis of SOM-MOFs, offering a versatile and high-yielding protocol. The enhanced stability and performance of SOM-MIL-88A highlight its potential for practical applications in adsorption, catalysis, enzyme immobilization, and biosensing.
A Universal Approach for High-Yield Synthesis of Single-Crystalline Ordered Macro-Microporous Metal−Organic Frameworks
Authors: Zhiqiang Zou, Zhuoyang Du, Lingmei Dai, Dehua Liu, Wei Du
DOI: 10.1021/jacs.4c11243
Link: https://pubs.acs.org/doi/10.1021/jacs.4c11243
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