Low-temperature catalytic oxidative desulfurization by two-phase system with O-bridged diiron perfluorophthalocyanine. (15th December 2021)

• Record Type: Journal Article
• Authors: Fang, Ze; Zhao, Zhiguo; Li, Nan; Zhu, Zhexin; Lu, Wangyang; Chen, Fengtao; Chen, Wenxing
• Is Part Of: Fuel. Volume 306(2021)
• Publication Date: 2021-12-15
• Subjects: Metallophthalocyanines -- Extractive desulfurization -- Oxidative desulfurization -- Dibenzothiophene -- High-valent iron-oxo; Fuel -- Periodicals; Coal -- Periodicals; Coal; Fuel; Periodicals; 662.6
• DOI: 10.1016/j.fuel.2021.121649
• Languages: English
• ISSNs: 0016-2361

Abstract

Graphical abstract: Highlights: An efficient extractive catalytic oxidation desulfurization system was developed. FePcF16 -O-FePcF16 exhibited excellent ODS performance at room temperature. A mixed solvent of ethanol and water was used as a "green" extractant. High-valent iron(IV)-oxo specie was the active species in the ODS process. Abstract: An environmentally friendly desulfurization technology was constructed innovatively through coupling extraction and oxidation technique under mild conditions. A biomimetic catalytic system was built by O-bridged diiron perfluorophthalocyanine (FePcF16 -O-FePcF16 ) and hydrogen peroxide, and its displayed excellent catalytic activity and satisfactory regenerative performance for the oxidative desulfurization reaction. A mixed solvent of ethanol and water (volume ratio 9:1) was used as a "green" extractant with the property of low cost and low toxicity. It was found that 99% of the conversion rate of dibenzothiophene was achieved successfully after 2 h operation at 30 °C. The catalyst system was cycled 6 times without significantly reducing the removal of DBT. The catalytic activity was in the order of dibenzothiophene > 4, 6-dimethyldibenzothiophene > benzothiophene. In addition, a possible reaction mechanism of the extraction and oxidative desulfurization was proposed and confirmed by electron paramagnetic resonance tests, gas chromatograph-mass spectrometer and electrospray ionization–mass spectrometry. The results demonstrated that the high-valent iron-oxo (Fe(IV) = O) was the main active species and this technology provides a novel idea for the design of high-efficiency, energy-saving and environmentally friendly desulfurization system.