Hexacyanoferrate-based ionic liquids as Fenton-like catalysts for deep oxidative desulfurization of fuels

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• 作者：Wei Jiang ; Hongping Li ; Sheng Yin ; Xin Wang ; Wei Liu ; Hui Liu ; Wenshuai Zhu and Huaming Li
• 刊名：Applied Organometallic Chemistry
• 出版年：2016
• 出版时间：September 2016
• 年：2016
• 卷：30
• 期：9
• 页码：753-758
• 全文大小：718K
• ISSN：1099-0739

文摘

Two hexacyanoferrate-based erm6">ionic liquids, [C₄Py]₃Fe(CN)₆ and [C₁₆Py]₃Fe(CN)₆, were synthesized and characterized using Fourier transform infrared and mass spectroscopies and CHN analysis. They were employed as Fenton-like catalysts in extraction and catalytic oxidative erm4">desulfurization of model oil with er" xmlns:mml="http://www.w3.org/1998/Math/MathML" id="aoc3500-eo-2000">erm2 TH_term3">dibenzothiophene (DBT), er" xmlns:mml="http://www.w3.org/1998/Math/MathML" id="aoc3500-eo-2001">erm3">benzothiophene (BT), er" xmlns:mml="http://www.w3.org/1998/Math/MathML" id="aoc3500-eo-2002">erm3">4,6-dimethyldibenzothiophene (4,6-DMDBT), er" xmlns:mml="http://www.w3.org/1998/Math/MathML" id="aoc3500-eo-2003">erm3">4-methyldibenzothiophene (4-MDBT) and er" xmlns:mml="http://www.w3.org/1998/Math/MathML" id="aoc3500-eo-2004">erm3">3-methylbenzothiophene (3-MBT) as substrates. Various polar solvents, such as erm6">ionic liquids, water and organic solvents, were applied to choose a suitable extractant. The results showed the removal of DBT reached 97.1% with [C₄Py]₃Fe(CN)₆ as a catalyst and er" xmlns:mml="http://www.w3.org/1998/Math/MathML" id="aoc3500-eo-2005">erm3">1-n-octyl-3-methylimidazolium hexafluorophosphate ([C₈mim]PF₆) as an extractant under optimal conditions. The activity of erm6">sulfur removal followed the order DBT > 3-MBT > BT > 4-MDBT >4,6-DMDBT. The effect of water content on erm6">sulfur removal was investigated by adding various concentrations of H₂O₂. It was found that excess water had a positive effect on erm6">sulfur removal but the catalysts were less sensitive than [FeCl₄⁻]-based catalysts to water. The mechanism was studied using electron spin-resonance spectroscopy and gas chromatography–mass spectrometry. O₂^•− may be the active oxygen species in the catalytic oxidative erm4">desulfurization process and the oxidation products of various erm6">sulfur compounds were the corresponding sulfoxides and sulfones. Copyright