A size-matched POM@MOF composite catalyst for highly efficient and recyclable ultra-deep oxidative fuel desulfurization†,Inorganic Chemistry Frontiers

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A size-matched POM@MOF composite catalyst for highly efficient and recyclable ultra-deep oxidative fuel desulfurization†
Inorganic Chemistry Frontiers ( IF 6.1 ) Pub Date : 2018-04-25 00:00:00 , DOI: 10.1039/c8qi00295a
Yun-Lei Peng _{1,

2,

3,

4} , Jingyi Liu _{1,

2,

3,

4} , Hai-Feng Zhang _{1,

2,

3,

4} , Dong Luo _{4,

5,

6,

7} , Dan Li _{4,

5,

6,

7}

Affiliation

A composite of Keggin-type phosphotungstic acid (H₃PW₁₂O₄₀) encapsulated in sized-matched metal–organic framework UiO-67 (PW₁₂@UiO-67) was prepared as a heterogeneous catalyst for extractive and catalytic oxidative desulfurization systems (ECODS). The appropriate cage size and narrow windows of UiO-67 serve to avoid the leaching of phosphotungstic acid, and also allow most sulfur compounds commonly found in fuels to approach the catalyst. The as-synthesized composite catalyst was characterized by powder X-ray diffraction (PXRD), Fourier transform infrared spectroscopy (FT-IR), thermogravimetric analysis (TGA), energy dispersive spectroscopy (EDS), and N₂ adsorption–desorption isotherms to confirm that PW₁₂ was successfully encapsulated in UiO-67 and the structure of UiO-67 was retained after immobilization. The obtained composite was examined as a heterogeneous catalyst in ECODS and showed remarkably high catalytic activity in the ultra-deep oxidative desulfurization of three sulfur compounds (benzothiophene, dibenzothiophene, and 4,6-dimethyldibenzothiophene) under mild conditions. The sulfur removal from 1000 ppm model oil reached 99.5% within 1 h at 70 °C for dibenzothiophene. The composite catalyst PW₁₂@UiO-67 could be easily regenerated and recycled for eight consecutive cycles without significant loss in catalytic activity.

中文翻译：

尺寸匹配的POM @ MOF复合催化剂，可实现高效且可回收的超深度氧化燃料脱硫†

封装在尺寸匹配的金属有机骨架UiO-67（PW ₁₂ @ UiO-67）中的Keggin型磷钨酸（H ₃ PW ₁₂ O ₄₀）复合材料被用作萃取和催化氧化脱硫系统的非均相催化剂（ ECODS）。UiO-67的适当笼尺寸和狭窄窗口可避免磷钨酸的浸出，并且还可以使燃料中常见的大多数硫化合物接近催化剂。粉末X射线衍射（PXRD），傅立叶变换红外光谱（FT-IR），热重分析（TGA），能量色散光谱（EDS）和N ₂吸附-解吸等温线表征了合成后的复合催化剂。那个PW_将12成功地封装在UiO-67中，并在固定后保留UiO-67的结构。所得复合物在ECODS中作为非均相催化剂进行了测试，在温和的条件下，在三种硫化合物（苯并噻吩，二苯并噻吩和4,6-二甲基二苯并噻吩）的超深度氧化脱硫中表现出极高的催化活性。对于二苯并噻吩，在70°C下1 h内从1000 ppm模型油中脱硫达到99.5％。复合催化剂PW₁₂ @ UiO-67可以很容易地再生和循环使用八个连续周期，而催化活性没有明显损失。

更新日期：2018-04-25

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