發(fā)布時間：2018-03-01 13:12

  本文關(guān)鍵詞： 脫硫 乳化 Janus納米片 破乳 循環(huán)利用　出處：《遼寧大學(xué)》2017年碩士論文　論文類型：學(xué)位論文

【摘要】：Janus乳化是基于其功能性分區(qū)的表面對兩相不互溶體系同時具有相親性而形成的乳化現(xiàn)象。與微乳化不同之處在于Janus乳化劑多為固態(tài)的Janus材料,其不僅可以實現(xiàn)兩相不互溶體系的有效乳化,而且通過簡單的操作,如離心,即可實現(xiàn)破乳,乳化劑亦可重復(fù)使用。本文成功合成出一系列兼具乳化劑和催化劑雙重功能的離子液體基Janus納米片,并首次將其應(yīng)用于燃油氧化脫硫體系,實現(xiàn)了模型油的深度氧化脫硫。離子液體基Janus納米片的制備,首先采用Pickering乳液界面材料化法,以三種硅烷化試劑為前驅(qū)體得到一側(cè)為親水基團的咪唑啉基,而另外一側(cè)為親油的苯基修飾的Janus石蠟球。利用四氫呋喃對石蠟良好的溶解性將石蠟內(nèi)核溶解后得到Janus中空球,進一步通過細胞超聲粉碎機粉碎,最終得到了咪唑啉基Janus納米片。其次,通過氯代正丁烷與Janus片上咪唑啉基之間的離子交換反應(yīng),制備了陰離子為Cl-的離子液體基Janus納米片。最后,利用離子交換反應(yīng),將[HSO4]-、[SiW12O40]4-、[PMo12O40]3-以及[PW12O40]3-引入到離子液體基Janus納米片上,從而得到了一種兼具催化劑和乳化劑雙功能的新型離子液體基Janus納米片。通過SEM、EDS、FT-IR以及XPS對其進行表征,結(jié)果表明四種酸根離子被成功固載到離子液體基Janus納米片上。分別以四種離子液體基Janus納米片為固體乳化劑對離子液體[BMIM]BF4和正辛烷進行乳化性能分析。結(jié)果顯示四種離子液體基Janus納米片均能將離子液體[BMIM]BF4和正辛烷乳化,并形成穩(wěn)定的乳液體系。通過光學(xué)電子顯微鏡可明顯觀察到乳液液滴的存在。本文首次將四種離子液體基Janus納米片應(yīng)用于燃油氧化脫硫體系,并實現(xiàn)了模型油的深度氧化脫硫。結(jié)果表明:[BMIM]3PMo12O40基Janus納米片為脫硫體系最佳催化劑。實驗確定了最佳反應(yīng)條件:催化劑用量為30 mg,O/S=5,T=50℃。在此基礎(chǔ)上考查了[BMIM]3PMo12O40基Janus納米片的脫硫性能。結(jié)果表明:當(dāng)反應(yīng)進行到1.5小時,二苯并噻吩(DBT)脫硫率達到100%,且進行六次循環(huán)利用,DBT的脫硫率依然能達到99.8%,無明顯下降。
[Abstract]:The emulsification of Janus is based on the fact that the surface of its functional partition is compatible with the two-phase immiscible system, which is different from microemulsification in that the Janus emulsifiers are mostly solid-state Janus materials. It can not only realize the effective emulsification of two-phase insoluble system, but also realize demulsification by simple operation, such as centrifugation. In this paper, a series of ionic liquid-based Janus nanoparticles with dual functions of emulsifier and catalyst have been successfully synthesized and applied to the fuel oil oxidation desulfurization system for the first time. Deep oxidation desulfurization of model oil was realized. Imidazoline group with hydrophilic group on one side was obtained by Pickering emulsion interfacial material method. On the other side, the oil-friendly phenyl modified Janus paraffin spheres were obtained by using the good solubility of tetrahydrofuran to dissolve the paraffin core to obtain the Janus hollow spheres, which were further crushed by a cellular ultrasonic pulverizer. Finally, Imidazolinyl Janus nanoparticles were obtained. Secondly, ionic liquid-based Janus nanoparticles with anions as Cl- were prepared by ion exchange reaction between chloro-n-butane and Imidazoline groups on Janus tablets. Finally, ion exchange reaction was used. [HSO4] -, [SiW12O40] 4, [PMo12O40] 3- and [PW12O40] 3- were introduced into ionic liquid-based Janus nanoparticles, and a novel ionic liquid-based Janus nanochip with dual functions of catalyst and emulsifier was obtained, which was characterized by SEM-EDSFT-IR and XPS. The results showed that four kinds of acid ions were successfully immobilized on the ionic liquid-based Janus nanoparticles, and the emulsifying properties of the ionic liquids [BMIM] BF4 and n-octane were analyzed using four kinds of ionic liquid-based Janus nanoparticles as solid emulsifiers respectively. The results showed that the emulsifying properties of the ionic liquids [BMIM] BF4 and n-octane were analyzed. Four kinds of ionic liquid-based Janus nanoparticles can emulsify the ionic liquid [BMIM] BF4 and n-octane. The existence of emulsion droplets can be observed by optical electron microscope. In this paper, four kinds of ionic liquid-based Janus nanoparticles were first used in the fuel oil oxidative desulfurization system. The results show that [BMIM] 3PMo12O40-based Janus nanoparticles are the best catalyst for desulfurization system. The optimum reaction conditions are determined as follows: the amount of catalyst is 30 mg / O / S ~ (5) T ~ (+) ~ (50 鈩，

本文編號：1552075