ABSTRACT To preparation of ultra-clean gasoline fuel, a new amphiphilic nanocomposite (TBA-SiWMn@PVA) has been successfully synthesized by supporting sandwich-type silicotungstate polyoxometalate ((n-C4H9)4N)7H5Si2W18Mn4O68 (TBA-SiWMn) on polyvinylalcohol (PVA) as an efficient catalyst for catalytic oxidative desulphurization (CODS) of gasoline. The synthesized materials were characterized by means of elemental analysis, 113Mn NMR, 29Si NMR, XRD, SEM, FT-IR and UV–vis techniques. The catalytic activity of TBA-SiWMn@PVA nanocomposite was tested on real gasoline in the presence of CH3COOH/H2O2 as an oxidant and the results were compared with model sulphur compounds at the same conditions. The TBA-SiWMn@PVA nanocomposite was shown excellent catalytic performance and recoverability for ODS of gasoline with high yield. The effects of the reaction time, reaction temperature, dosage and nature of catalyst were investigated. The reaction mechanism and the kinetic parameters of sulphur compounds oxidation were also discussed. The probable mechanism was proposed via the electrophilic mechanism through the formation of a peroxometalate intermediate complex with phase transfer properties. Results were indicated that the kinetics of sulphur oxidation fitted the pseudo-first-order kinetic model. After 5 oxidation runs, the heterogeneous nanocatalyst was separated and recovered easily. GRAPHICAL ABSTRACT

中文翻译：

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使用两亲性多金属氧酸盐@聚合物纳米复合材料作为高效、可重复使用的绿色有机-无机杂化催化剂催化氧化脱硫汽油

摘要 为了制备超清洁汽油燃料，通过在聚乙烯醇（PVA）上负载夹心型硅钨酸多金属氧酸盐（（n-C4H9）4N）7H5Si2W18Mn4O68（TBA-SiWMn），成功合成了一种新型两亲纳米复合材料（TBA-SiWMn@PVA）。 ) 作为汽油催化氧化脱硫 (CODS) 的有效催化剂。通过元素分析、113Mn NMR、29Si NMR、XRD、SEM、FT-IR 和 UV-vis 技术对合成的材料进行了表征。在 CH3COOH/H2O2 作为氧化剂存在下，在真实汽油上测试了 TBA-SiWMn@PVA 纳米复合材料的催化活性，并将结果与​​相同条件下的模型硫化合物进行了比较。TBA-SiWMn@PVA 纳米复合材料对汽油的 ODS 具有优异的催化性能和可回收性，收率很高。反应时间的影响 考察了催化剂的反应温度、用量和性质。还讨论了硫化物氧化的反应机理和动力学参数。可能的机制是通过亲电机制通过形成具有相转移特性的过氧金属酸盐中间体复合物提出的。结果表明，硫氧化动力学符合准一级动力学模型。经过 5 次氧化运行后，多相纳米催化剂很容易分离和回收。图形概要 可能的机制是通过亲电机制通过形成具有相转移特性的过氧金属酸盐中间体复合物提出的。结果表明，硫氧化动力学符合准一级动力学模型。经过 5 次氧化运行后，多相纳米催化剂很容易分离和回收。图形概要 可能的机制是通过亲电机制通过形成具有相转移特性的过氧金属酸盐中间体复合物提出的。结果表明，硫氧化动力学符合准一级动力学模型。经过 5 次氧化运行后，多相纳米催化剂很容易分离和回收。图形概要