Keggin型磁性多酸负载型催化剂的制备及其燃油氧化脱硫性能  

Preparation of Keggin-Type Magnetic Heteropolyacid Supported Catalyst and Their Oxidative Desulfurization Performance for Fuel

作　　者：李斯文 张海艳[1] 韩天昊 吴文琪 王伟[1] 赵建社[2] LI Siwen;ZHANG Haiyan;HAN Tianhao;WU Wenqi;WANG Wei;ZHAO Jianshe(School of Water and Environment, Chang’an University, Xi’an 710061, China;College of Chemistry & Material Science, Northwest University, Xi’an 710127, China)

机构地区：[1]长安大学水利与环境学院,陕西西安710061 [2]西北大学化学与材料科学学院,陕西西安710127

出　　处：《石油学报（石油加工）》2022年第1期37-45,共9页Acta Petrolei Sinica(Petroleum Processing Section)

基　　金：国家自然科学基金项目(21671157);长安大学中央高校基本科研业务(300102290301)资助。

摘　　要：采用简单的一锅法合成了一类氨基修饰的磁性MIL-101(Cr)载体固载下的Keggin型多酸催化剂,即Fe3O4@MIL-101-PMoW(简称FeCuP),通过傅里叶变换红外光谱(FT-IR)、X射线衍射(XRD)、N2吸附-脱附等温(BET)以及振动样品磁强计(VSM)等手段对其组成、形貌等进行表征。采用该催化剂催化以空气中的氧气为氧化剂、以二苯并噻吩(DBT)为硫源的正十二烷模拟油样。结果表明,多酸具有较好的脱硫效果,随着多酸活性组分的引入,在最优反应条件下,FeCuP催化氧化模拟燃油中DBT的脱硫率可在75 min内达到100%。此外,磁性材料的修饰可大大增加FeCuP催化剂的回收率,采用简单的外加磁场即可实现催化剂的回收与再利用,重复使用10次以上仍保持95%以上的脱硫率。FeCuP催化剂在脱硫率以及重复使用次数上的明显优化满足了当今脱硫工业化的使用要求,具有较大的利用及推广价值。A kind of loaded Keggin heteropolyacid catalysts with the amino modified magnetic MIL-101(Cr)as carrier has been obtained under a simple one pot synthesis method,namely Fe3O4@MIL-101-PMoW(hereinafter referred to as FeCuP).Fourier transform infrared spectroscopy(FT-IR),X-ray diffraction(XRD),N2 adsorption stripping isothermal curve(BET),Vibrating sample magnetometer(VSM)and so on,have been used to characterize the composition and morphology.Using the FeCuP as catalyst and oxygen in the air as oxidant to catalytic oxidation of the simulate oil samples,in which dibenzothiophene(DBT)as sulfur source,the results show a good desulfurization effect.With the introduction of the active components of heteropolyacids,the desulfurization rate of DBT in simulated fuel oil can reach 100%within 75 min under the optimal reaction conditions.In addition,the catalyst recovery times can be greatly increased by the modification of magnetic materials.The recovery and reuse can be realized by using a simple external magnetic field.The desulfurization rate can be maintained above 95%after repeated use for more than 10 times.The optimization of desulfurization rate and the times of repeated use of this kind of catalyst can meet the requirements of desulfurization industrialization,even the great utilization and popularization value.

关 键 词：杂多酸 磁性材料 氧化脱硫 重复使用 二苯并噻吩 

分 类 号：TB333[一般工业技术—材料科学与工程]