Zhaojin Zhang,Yinan Li,Jing Gao,Alula Yohannes,Hang Song,Shun Yao
Based on above background, quinolinium, 8-hydroxy-quinolinium, and benzothiazolium ionic liquids, containing the acidic anions of methanesulfonate ([CH3SO3]−), phosphate ([H2PO4]−),p-toluenesulfonate ([p-TSA]−), and bisulfate ([HSO4]−) were synthesized. After comparison, the aqueous solution of benzothiazole bisulfate [HBth][HSO4] was selected as the most ideal extractant for removing pyridine and aniline. Meanwhile, benzothiazole bisulfate [HBth][HSO4] solution was found as the best one for removing quinoline from simulated oil. Then, the single stage extraction and two-step extraction were used in the extraction for the simulated oil containing pyridine, quinoline or aniline, and their mixture, respectively. Their denitrogenation performance on their N-removal effect was compared on the basis of structural features, and main extraction conditions were further investigated, including mass ratio of IL to water, mass ratio of IL to oil, and temperature. Furthermore, the extraction process was described by two kinetic equations. Recovery and reuse of IL were realized by back-extraction and liquid-liquid separation, and a related mechanism was speculated, according to all the experimental results. Finally, based on the developed method for preparing complex adsorbent tablets, corresponding immobilized IL was used to remove target objects, by solid phase extraction, in order to extend separation ways, which was more easily recovered after extraction.Keywords:ionic liquids;denitrogenation;extraction;pyridine;quinoline;aniline;simulated oil
In this work, the study of synthesis and denitrogenation of magnetic polymeric ionic liquids (PILs) for N-compounds in simulated oils and diesel are reported. Three functionalised magnetic particles, Fe 3 O 4 @SiO 2 @PILs with side alkyl chain of C2, C4 and C6, respectively, were prepared by grafting PILs on the surface of silica-coated Fe 3 O 4 . Fourier transform infrared spectra, thermogravimetric analysis, X-ray diffraction and scanning electron microscopy were carried out to characterise the structure of Fe 3 O 4 @SiO 2 @PILs. It has shown that Fe 3 O 4 @SiO 2 @ PILs possess precious merits for sorbents, such as regular morphology, good stability and magnetic properties. Denitrogenation experiments of simulated oils demonstrate that Fe 3 O 4 @SiO 2 @ PILs show better denitrogenation efficiency of basic N-compounds than neutral N-compounds. The effects of temperature, reaction times, ratio of reagent to oil on denitrogenation for simulated oils were explored, and 92.1% denitrogenation efficiency was obtained to remove quinoline from simulated oils. Denitrogenation of Fe 3 O 4 @SiO 2 @PILs in diesel leads to 84.3% denitrogenation efficiency, and it can remain 82.5% denitrogenation efficiency after five times of recycles. Compared with other similar sorbents, Fe 3 O 4 @SiO 2 @PILs show competitive performances to eliminate organic N-compounds. It is hopeful that Fe 3 O 4 @SiO 2 @PILs can be promising sorbents for purification of liquid fuel by adsorptive denitrogenation.
Here, a hydrophilic fumed silica (F-SiO2) was used as a support, and we place phosphotungstic acid (HPW) onto the F-SiO2 via a simple impregnation method normally used to prepare a HPW/F-SiO2 catalyst, which is used in oxidative desulfurization processes. A number of characterization analyses were used, such as X-ray diffraction, Fourier transform infrared, and Transmission electron microscopy, to prove that the HPW catalyst was homogeneously distributed on the F-SiO2. The structural parameters of the catalyst and the support were tested with Brunauer–Emmett–Teller, and it was confirmed that the catalyst is a mesoporous material. Energy-dispersive spectrometry was used to characterize the distribution of the active component distribution. Catalytic performance was investigated using the catalytic oxidative desulfurization process. During optimal conditions, the removal effect of dibenzothiophene (DBT) in simulated oil can reach 100%. After 13 cycles, catalytic activity is still high, and the DBT conversion can still attain 95.362%.
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