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首页> 外文期刊>Catalysis science & technology >An efficient oxidative desulfurization process using terbium-polyoxometalate@MIL-101 (Cr)
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An efficient oxidative desulfurization process using terbium-polyoxometalate@MIL-101 (Cr)

机译：使用Terbium-Polyoxemometate@MIL-101（CR）进行有效的氧化脱硫过程

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An efficient and recyclable oxidative desulfurization process (ODS) to remove the most refractory sulfurcompounds (dibenzothiophene, 1-benzothiophene and 4,6-dimethyldibenzothiophene) from fuel is reported. The ODS process was catalyzed by terbium-polyoxometalate [Tb(PWi_(11)O~(39))2]~(11-) (Tb(PW_(11))2) and its composite Tb(PW_(11))2@MIL-101. The tetrabutylammonium (TBA) salt of Tb(PW_(11))2 was prepared and further incorporated in the porous metal-organic framework MIL-101(Cr). The TBA compound and its composite were characterized by various techniques (powder X-ray diffraction, FT-IR, FT-Raman, SEM and elemental analysis), and their electrochemical behavior was investigated, indicating that the structure of the polyoxometalate anion must be retained after immobilization, The studied ODS process was based on a biphasic system formed by a model oil with various refractor sulfur-compounds and an extracting solvent using H2O2 as the oxidant. Two main steps in the process were carefully investigated: the initial extraction and the oxidative catalytic stage. The optimization of the ODS process was performed by the analysis of the most suitable extracting solvent and also comparing the desulfurization performance of the homogeneous Tb(PW_(11))2 and the heterogeneous Tb(PW_(11))2@MIL-101 catalysts. Acetonitrile was selected as the best solvent because it allowed the highest desulfurization rate, conciliating good initial extraction and high catalytic performance. The presence of the porous catalyst Tb(PW_(11))2@MIL-101 seemed not to influence the initial extraction step; however, with this porous hybrid catalyst were obtained higher desulfurization rates during the catalytic stage. Remarkably, using Tb(PW_(11))2@MIL-101 and the oil-acetonitrile system complete desulfurization of oil was achieved only after 5 h. The recyclability of the solid catalyst was investigated for three consecutive ODS cycles and its stability was confirmed by several techniques.
机译：据报道，从燃料中，一种有效且可回收的氧化脱硫过程（ODS）可从燃料中清除最难治性的硫共硫酸盐（Dibenzothiophene，1-苯并噻吩和4,6-二甲基苯乙烯）。 ODS过程是由terbium-polyoxemometalate [TB（PWI_（11）O〜（39））2]〜（11-）（TB（PW_（11））2）及其复合TB（PW_（11）2）催化的ODS过程。 @MIL-101。制备了TB（PW_（11））2的四丁丁基铵（TBA）盐，并进一步掺入多孔金属有机框架MIL-101（CR）中。 TBA化合物及其复合材料的特征是各种技术（粉末X射线衍射，FT-IR，FT-RAMAN，SEM和元素分析），并研究了它们的电化学行为，表明必须保留多氧阴离子的结构固定后，研究的ODS过程基于由具有各种折射硫化合物的模型油形成的双相系统，并使用H2O2作为氧化剂提取溶剂。仔细研究了该过程中的两个主要步骤：初始提取和氧化催化阶段。 ODS过程的优化是通过分析最合适的提取溶剂的分析，并比较了均质TB（PW_（11））2和异质TB（PW_（11））2@MIL-101催化剂的脱硫性能。乙腈被选择为最佳溶剂，因为它允许最高的脱硫化速率，调解良好的初始提取和高催化性能。多孔催化剂TB（PW_（11））2@MIL-101的存在似乎不影响初始提取步骤。然而，在催化阶段，获得了这种多孔杂化催化剂的脱硫速率。值得注意的是，仅使用TB（PW_（11））2@MIL-101，并且仅在5小时后才能实现石油 - 乙腈系统的完全脱硫。研究了三个连续的OD循环的固体催化剂的可回收性，并通过多种技术证实了其稳定性。

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