Extractive/catalytic oxidative mechanisms over [Hnmp]Cl center dot xFeCl(3) ionic liquids towards the desulfurization of model oils

摘要

In this work, N-methyl-2-pyrrolidonium (NMP) was acidized using hydrochloric acid to obtain [Hnmp]Cl first, which was then reacted with FeCl3 to prepare a series of inexpensive tunable [Hnmp]ClxFeCl(3) (x = 0.2-2.0) ionic liquids (ILs) for the extractive and oxidative desulfurization of model oils. The Lewis acidities of these ILs were tested by the Fourier transform infrared (FT-IR) method, which indicated that when the x value of [Hnmp]ClxFeCl(3) was above 1.0, the ILs exhibited Lewis acidity. The extraction results showed that the acidification of NMP reduced its dissolubility ability toward dibenzothiophene (DBT) and its Lewis acidity played a determining role in extractive desulfurization. In the catalytic oxidation removal process of the DBT model oil in the presence of H2O2, electron paramagnetic resonance (EPR) and scavenger experiments showed that the hydroxyl radical (OH) plays a key role and the superoxide anion radical (O-2(-)) has a minor function. [Hnmp]Cl1.5FeCl(3) IL showed excellent recycling performance, which was due to its high dissolving capacity (23700 ppm) for dibenzothiophene-sulfone (DBTO2).