通过质子离子液体的双重活化作用对模型柴油进行氧化脱硫。
Oxidative desulfurization of model diesel via dual activation by a protic ionic liquid.
机构信息
Green Chemistry Centre, College of Chemistry and Chemical Engineering, Yantai University, Yantai, 264005, China.
Green Chemistry Centre, College of Chemistry and Chemical Engineering, Yantai University, Yantai, 264005, China.
出版信息
J Hazard Mater. 2014 Aug 30;279:220-5. doi: 10.1016/j.jhazmat.2014.07.005. Epub 2014 Jul 15.
A novel and green carboxylate-anion-based protic ionic liquid (PIL), [Hnmp]HCOO, was prepared through a simple and atom economic neutralization reaction between N-methyl-2-pyrrolidonium (NMP) and formic acids. Both FT-IR spectra and (1)H NMR confirmed its simple salt structure. [Hnmp]HCOO exhibited so high catalytic activity that the dibenzothiophene (DBT) removal reached 99% at 50°C in 3h under conditions of VPIL/Vmodel oil=1:10 and H2O2/DBT (O/S, molar ratio)=5. The catalytic oxidation reactivity of S-compounds was found to be in the order of DBT>4,6-dimethyldibenzothiophene (4,6-DMDBT)>benzothiophene (BT). The investigation on mechanism showed that oxidative desulfurization was realized through dual activation of PIL. Moreover, [Hnmp]HCOO can be recycled for five times with an unnoticeable decrease in desulfurization activity.
一种新型的、基于羧酸阴离子的绿色质子离子液体[Hnmp]HCOO 通过 N-甲基-2-吡咯烷酮（NMP）和甲酸之间的简单原子经济性中和反应制备而成。FT-IR 光谱和 1H NMR 都证实了其简单的盐结构。[Hnmp]HCOO 表现出很高的催化活性，在 VPIL/Vmodel oil=1:10 和 H2O2/DBT（O/S，摩尔比）=5 的条件下，在 50°C 下 3 小时内，二苯并噻吩（DBT）的去除率达到 99%。发现 S 族化合物的催化氧化反应活性顺序为 DBT>4,6-二甲基二苯并噻吩（4,6-DMDBT）>苯并噻吩（BT）。对机理的研究表明，通过 PIL 的双重活化实现了氧化脱硫。此外，[Hnmp]HCOO 可以回收五次，脱硫活性没有明显下降。
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