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Designing multifunctional SO3H-based polyoxometalate catalysts for oxidative desulfurization in acid deep eutectic solvents

机译:设计多功能SO3H基多氧酸盐催化剂,用于酸深凝胶溶剂中的氧化脱硫

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摘要

Deep eutectic solvents (DESs) are 'green' sustainable solvents with wide applications such as extractive desulfurization of fuel; however, their low extraction efficiency is a major limitation to such applications. In this work, several SO3H-functionalized polyoxometalates were prepared and applied to oxidative desulfurization of fuels with acidic DESs as extractants and 30 wt% of H2O2 as an oxidant. Compared with neutral POM catalysts, acidic catalysts, such as [PSTEtA]3PW(12)O(40), exhibited higher catalytic performance with 100% desulfurization efficiency. However, in the absence of DESs sulfur removal was only 9.6% with [PSTEtA](3)PW12O40 used as a catalyst. To study the role of the DESs, three types of DESs were evaluated on extraction and oxidation of dibenzothiophene (DBT), with acidic DES ChCl/2Ac exhibiting the best performance. The effects of different reaction conditions, such as the amount of H2O2 and ChCl/2Ac, reaction temperature and time, different sulfur compounds, and fuel composition, were investigated. Combined with the kinetic study, results suggested that oxidation of DBT was attributed to a pseudo-first-order kinetic reaction. The activities of different sulfur compounds decreased in the order of DBT 3-methylbenzothiophene (3-MBT) 4-methyldibenzothiophene (4-MDBT) 4,6-dimethyldibenzothiophene (4,6-DMDBT) benzothiophene (BT). Compared with aromatics, the sulfur removal could be strongly affected by olefins, showing a drop of up to 66.6%.
机译:深度共晶溶剂(DESS)是“绿色”可持续溶剂,具有广泛的应用,如燃料的萃取脱硫;然而,它们的低提取效率是对这些应用的重大限制。在这项工作中,制备几种SO 3官能化的多氧化血酸盐并用酸性DES作为萃取剂和30wt%的H 2 O 2作为氧化剂氧化脱硫。与中性POM催化剂相比,酸性催化剂,例如[PSTETA] 3PW(12)O(40),表现出具有100%脱硫效率的催化性能。然而,在没有DESS硫的情况下,用用作催化剂的[PSTETA](3)PW12O40仅为9.6%。为研究DES的作用,评价三种类型的DES是对二苯并噻吩(DBT)的提取和氧化,酸性DES CHCL / 2AC表现出最佳性能。研究了不同反应条件的影响,例如H 2 O 2和CHCl / 2Ac的量,反应温度和时间,不同的硫化合物和燃料组合物。结合动力学研究,结果表明,DBT的氧化归因于伪一阶动力学反应。不同硫化合物的活性按DBT&GT的顺序减少; 3-甲基苯并噻吩(3-MBT)& 4-甲基二苯甲酸噻吩(4-MDBT)> 4,6-二甲基二苯甲酸噻吩(4,6-DMDBT)>苯并噻吩(BT)。与芳烃相比,硫去除可能受烯烃的强烈影响,显示出高达66.6%的滴度。

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  • 来源
    《RSC Advances》 |2017年第87期|共8页
  • 作者单位

    Jiangsu Univ Inst Energy Res 301 Xuefu Rd Zhenjiang 212013 Peoples R China;

    Jiangsu Univ Sch Chem &

    Chem Engn 301 Xuefu Rd Zhenjiang 212013 Peoples R China;

    Jiangsu Univ Sch Chem &

    Chem Engn 301 Xuefu Rd Zhenjiang 212013 Peoples R China;

    Jiangsu Univ Sch Chem &

    Chem Engn 301 Xuefu Rd Zhenjiang 212013 Peoples R China;

    Jiangsu Univ Inst Energy Res 301 Xuefu Rd Zhenjiang 212013 Peoples R China;

    Jiangsu Univ Inst Energy Res 301 Xuefu Rd Zhenjiang 212013 Peoples R China;

    Jiangsu Univ Sch Chem &

    Chem Engn 301 Xuefu Rd Zhenjiang 212013 Peoples R China;

    Jiangsu Univ Inst Energy Res 301 Xuefu Rd Zhenjiang 212013 Peoples R China;

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  • 原文格式 PDF
  • 正文语种 eng
  • 中图分类 化学;
  • 关键词

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