Creation of Active Sites in MOF‐808(Zr) by a Facile Route for Oxidative Desulfurization of Model Diesel Oil,ChemistrySelect

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Creation of Active Sites in MOF‐808(Zr) by a Facile Route for Oxidative Desulfurization of Model Diesel Oil
ChemistrySelect ( IF 1.9 ) Pub Date : 2020-01-02 , DOI: 10.1002/slct.201903376
Yulong Gu ₁ , Gan Ye ₁ , Wei Xu ₂ , Wei Zhou ₃ , Yinyong Sun ₁

Affiliation

MOF‐808(Zr) as an important member of metal‐organic frameworks (MOFs) has attracted much attention due to its good stability, large surface area and rich zirconium metal centers. However, Zr sites in the structure of MOF‐808(Zr) are inactive in many catalytic reactions due to they are well coordinated with organic ligands like 1,3,5‐benzenetricarboxylic acid (BTC) and formate anions. Thus, removing formate anions have been attempted to create more active sites in the structure for many reactions while maintaining the structural stability. In this work, we report that the formate ligands in MOF‐808(Zr) can be facilely removed by the treatment in hot ethanol for 4 h. The obtained material as a heterogeneous catalyst exhibited superior catalytic activity in the oxidative desulfurization (ODS) reaction of dibenzothiophene (DBT) compared with reported MOFs catalysts. The conversion of DBT in model diesel oil could reach >99 % within a reaction time of 20 min at 323 K, which is five times as that over parent MOF‐808(Zr). As a result, the sulfur content was decreased from 1000 ppm to less than 10 ppm. Such catalytic performance should be mainly attributed to the creation of more active sites in the structure of MOF‐808(Zr) after the removal of formate anions.

中文翻译：

在MOF-808（Zr）中通过模型柴油氧化脱硫的简便途径创建活性位点

MOF-808（Zr）作为金属有机框架（MOF）的重要成员，因其良好的稳定性，较大的表面积和丰富的锆金属中心而备受关注。但是，MOF-808（Zr）结构中的Zr位在许多催化反应中均无活性，因为它们与有机配体（如1,3,5-苯三甲酸（BTC）和甲酸根阴离子）很好地配合。因此，已经尝试除去甲酸根阴离子以在许多反应中在结构中产生更多的活性位点，同时保持结构的稳定性。在这项工作中，我们报告说，通过在热乙醇中处理4小时，可以轻松除去MOF-808（Zr）中的甲酸配体。与报道的MOFs催化剂相比，所获得的材料作为多相催化剂在二苯并噻吩（DBT）的氧化脱硫（ODS）反应中显示出优异的催化活性。在323 K下20分钟的反应时间内，模型柴油中DBT的转化率可达到> 99％，是母体MOF-808（Zr）的五倍。结果，硫含量从1000ppm降低至小于10ppm。这种催化性能应主要归因于除去甲酸根阴离子后，MOF-808（Zr）结构中产生了更多的活性位。

更新日期：2020-01-02

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