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Deep Oxidative Desulfurization of Planar Compounds Over Functionalized Metal-Organic Framework UiO-66(Zr): An
Bijan Barghi1, Tanel Mõistlik1, Anastassia Raag1
1Virumaa College School of Engineering, Tallinn University of Technology, Järveküla 75, Kohtla-Järve 30322, Estonia.
ACS Omega
|June 10, 2024
Summary
Ligand-modified UiO-66, particularly UiO-66-NO2, shows high efficiency in deep oxidative desulfurization of model fuels, removing up to 98.68% of dibenzothiophene. The catalysts demonstrate good reusability for fuel purification applications.
Area of Science:
- Materials Science
- Catalysis
- Environmental Chemistry
Background:
- Deep oxidative desulfurization is crucial for removing refractory sulfur compounds from fuels.
- Metal-organic frameworks (MOFs) offer tunable properties for catalytic applications.
- Functionalized UiO-66 MOFs are investigated for enhanced catalytic performance.
Purpose of the Study:
- To evaluate the catalytic activity and stability of ligand-modified UiO-66 in deep oxidative desulfurization.
- To compare the effectiveness of UiO-66 with different functional groups (-NO2, -OH) for sulfur removal.
- To optimize desulfurization conditions using statistical methodologies.
Main Methods:
- Synthesis and characterization of functionalized UiO-66 (MOF) using XRD, FTIR, NMR, SEM, TGA, and gas adsorption.
- Application of central composite design and response surface methodology for experimental optimization.
- Testing catalytic activity against planar sulfur compounds: dibenzothiophene (DBT), 2-methylbenzothiazole (2-MB), and 4,6-dimethyldibenzothiophene (4,6-DMDBT).
Main Results:
- UiO-66-NO2 exhibited the highest removal efficiency: 98.68% for DBT, 93.23% for 2-MB, and 69.32% for 4,6-DMDBT.
- Optimal conditions: 66.7 °C, 3.0 equiv oxidant, and 9.7 wt% catalyst loading.
- Sulfur compound oxidation followed the trend DBT > 2-MB >> 4,6-DMDBT.
- All tested MOFs showed acceptable catalytic activity and reusability over four cycles, with minor activity loss.
Conclusions:
- Ligand modification significantly impacts UiO-66's catalytic activity in deep oxidative desulfurization.
- UiO-66-NO2 is a highly effective catalyst for removing planar sulfur compounds from model fuels.
- The developed MOFs demonstrate potential for practical applications in fuel desulfurization due to their activity and reusability.
