Journal
CHEMICAL ENGINEERING JOURNAL
Volume 433, Issue -, Pages -Publisher
ELSEVIER SCIENCE SA
DOI: 10.1016/j.cej.2021.133569
Keywords
Extraction-oxidative desulfurization; O-bridged diiron perfluorophthalocyanine; 4-Mercaptopyridine; High-valentiron-oxo species
Categories
Funding
- National Natural Science Foundation of China [51703201]
- Zhejiang Provincial Natural Science Foundation of China [LQ17E030003]
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In this study, a novel composite catalyst FePcF16-O-FePcF16/4-Mpy was designed and prepared, showing enhanced catalytic activity through axial coordination. The catalyst exhibited high efficiency in extraction oxidative desulfurization, achieving a high desulfurization rate in a short period of time. Furthermore, the catalyst showed good stability after multiple cycles of use.
Developing efficient and environmentally friendly catalytic system is significant for the removal of sulfide in fuel. O-bridged diiron perfluorophthalocyanine/4-mercaptopyridine (FePcF16-O-FePcF16/4-Mpy) as a novel composite catalyst was designed and prepared by axial coordination. The catalyst characterization was conducted through ultraviolet-visible spectroscopy, fourier transform infrared spectroscopy, X-ray diffractometry, electrospray ionization-mass spectrometry and density-functional theory technology. A high-efficient extraction oxidative desulfurization system is composed of hydrogen peroxide (H2O2), the mixture of ethanol and water and FePcF16-O-FePcF16/4-Mpy. Notably, the coordination of 4-Mpy greatly enhanced the catalytic activity of FePcF16-O-FePcF16, 99.4% of the desulfurization rate was achieved in 20 min at 30?degrees C. The catalyst system was cycled 8 times without significantly reducing the removal of dibenzothiophene. Electron paramagnetic resonance and gas chromatography-mass spectroscopy proved the high-valent iron-oxo intermediates were the main active substances in the FePcF16-O-FePcF16/4-Mpy/H2O2 system, and the pathway of catalytic oxidation DBT was proposed. This work provided useful insights to select suitable ligands to improve the activity of metal phthalocyanine, and offered a novel idea for the construction of efficient oxidative desulfurization system.
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