Deep Oxidative Desulfurization of Fuel Catalyzed by Modified Heteropolyacid: The Comparison Performance of Three Kinds of Ionic Liquids,ACS Sustainable Chemistry & Engineering

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Deep Oxidative Desulfurization of Fuel Catalyzed by Modified Heteropolyacid: The Comparison Performance of Three Kinds of Ionic Liquids
ACS Sustainable Chemistry & Engineering ( IF 7.1 ) Pub Date : 2018-10-16 00:00:00 , DOI: 10.1021/acssuschemeng.8b04524
Si-Wen Li ₁ , Rui-Min Gao ₂ , Jian-she Zhao ₁

Affiliation

Three kinds of ionic-liquid (IL)-modified heteropolyacids, with one N atom, two N atoms, and cyclic N type of quaternary ammonium salt, were synthesized successfully (S-POM, D-POM, and C-POM), and the relative heterogeneous catalysts system for oxidative desulfurization was obtained from simple one-pot hydrothermal reaction and modified heteropolyacids in the pores of MCM-41 after MOF-199 template self-assembly (S/D/[email protected]@MCM-41). These as-designed samples were characterized via XRD, XPS, TEM, BET analysis, and so on. Results showed that the S/D/C-POM active species could be successfully immobilized into the mesoporous materials and all retained their Keggin structure. C-PMM carried out excellent performance for oxidesulfurization. Under optimal conditions, the rate of DBT removal could reach up to 100% in 90 min, and the catalyst was reused more than 10 times with nearly no significant reduction on catalytic activity. The various sulfur compounds also had an important effect on catalytic performance, which was also investigated and showed the competitive adsorption oxidation with the BT and 4,6-DMDBT in real oils from the DFT calculation. According to the real diesel oxidative desulfurization, it was found that nearly all the sulfur compounds could be completely removed. Meanwhile, a possible mechanism is also studied under the calculation evaluation.

中文翻译：

改性杂多酸催化燃料的深度氧化脱硫：三种离子液体的比较性能

成功合成了三种具有1个N原子，2个N原子和环状N型季铵盐的离子液体（IL）改性杂多酸（S-POM，D-POM和C-POM），并且MOF-199模板自组装后，通过简单的一锅水热反应和MCM-41孔中的改性杂多酸（S / D / [电子邮件保护] @ MCM-41）获得了用于氧化脱硫的相对多相催化剂体系。通过XRD，XPS，TEM，BET分析等对这些设计好的样品进行了表征。结果表明，S / D / C-POM活性物质可以成功地固定在介孔材料中，并且都保留了其Keggin结构。C-PMM在氧化物硫化方面表现出色。在最佳条件下，DBT去除率可在90分钟内达到100％，催化剂可重复使用10次以上，催化活性几乎没有明显降低。各种含硫化合物对催化性能也有重要影响，还进行了研究，并通过DFT计算显示了在真实油中BT和4,6-DMDBT具有竞争性吸附氧化作用。根据实际的柴油氧化脱硫，发现几乎所有的硫化合物都可以完全去除。同时，在计算评估中还研究了一种可能的机制。根据实际的柴油氧化脱硫，发现几乎所有的硫化合物都可以完全去除。同时，在计算评估中还研究了一种可能的机制。根据实际的柴油氧化脱硫，发现几乎所有的硫化合物都可以完全去除。同时，在计算评估中还研究了一种可能的机制。

更新日期：2018-10-16

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