School of Chemical Engineering and Technology, Tianjin University, Tianjin 300072, People's Republic of China.
School of Chemical Engineering and Technology, Tianjin University, Tianjin 300072, People's Republic of China.
J Hazard Mater. 2017 Jul 5;333:63-72. doi: 10.1016/j.jhazmat.2017.03.017. Epub 2017 Mar 10.
In this work, the simple preparation of novel polymer supported polyoxometallates (POMs) catalysts has been reported. Soluble task-specific cross-linked poly (ionic liquid) (PIL) was prepared with N,N-dimethyl-dodecyl-(4-vinylbenzyl) ammonium chloride and divinylbenzene as co-monomers. The as-prepared cationic PILs were assembled with different commercial POMs to form the interlinked mesoporous catalysts, and the formation mechanism was provided. The catalytic oxidation activities of the catalysts were closely related to the formation pathway of their corresponding peroxide active species. The catalyst with HWO as counterion, which exhibited the best activity in the oxidation of benzothiophene (BT) and dibenzothiophene (DBT) to sulfones in model oil with hydrogen peroxide (HO, 30wt%) as oxidant, was characterized by different techniques and systematically studied for its sulfur removal performance. As for the oxidative desulfurization of a real diesel, it was observed that almost all of the original sulfur compounds could be completely converted, and the catalyst could be reused for at least eight cycles without noticeable changes in both catalytic activity and chemical structure. In the end, a catalytic mechanism was put forward with the assistant of Raman analysis.
在这项工作中,我们报道了一种新型聚合物负载多金属氧酸盐(POMs)催化剂的简单制备方法。采用 N,N-二甲基-十二烷基-(4-乙烯基苄基)氯化铵和二乙烯基苯作为共聚单体,制备了可溶性的功能化交联聚(离子液体)(PIL)。所制备的阳离子 PIL 与不同的商业 POM 组装形成互穿介孔催化剂,并提供了其形成机制。催化剂的催化氧化活性与过氧化物活性物种的形成途径密切相关。以 HWO 为抗衡离子的催化剂在以过氧化氢(HO,30wt%)为氧化剂的模型油中氧化苯并噻吩(BT)和二苯并噻吩(DBT)生成砜的反应中表现出最好的活性,用不同的技术对其进行了表征,并对其脱硫性能进行了系统研究。对于实际柴油的氧化脱硫,观察到几乎所有原始的硫化合物都可以完全转化,并且催化剂可以至少重复使用八次,在催化活性和化学结构方面没有明显变化。最后,通过拉曼分析提出了一种催化机制。