新型磁性聚离子液体的合成及其油品脱氮性能研究
PDF下载 (445)时运生,李 杰,王 峰,张剑锋.新型磁性聚离子液体的合成及其油品脱氮性能研究[J].宁波大学学报(理工版),2019,32(4):94-101.DOI:
SHI Yunsheng,LI Jie,WANG Feng,ZHANG Jianfeng.Synthesis of novel magnetic poly(ionic liquids) and denitrification performance of fuel oil[J].Journal of Ningbo University(Natural Science & Engineering Edition),2019,32(4):94-101.DOI:
| Title: | Synthesis of novel magnetic poly(ionic liquids) and denitrification performance of fuel oil |
| 作者: | 时运生, 李 杰, 王 峰, 张剑锋 |
| Author(s): | SHI Yunsheng, LI Jie, WANG Feng, ZHANG Jianfeng |
| 关键词: | 四氧化三铁; 聚离子液体; 脱氮; 喹啉 |
| Keywords: | ferroferric oxide; poly(ionic liquids); denitrification; quinolone |
| 分类号: | TE624 |
| 文献标识码: | A |
| 摘要: | 将1-乙烯基-3-乙酸咪唑溴盐和磁性乙烯基硅烷进行自由基聚合反应, 再通过阴离子交换, 合成了3种不同阴离子的磁性聚离子液体Fe3O4@SiO2@PILs-X(X=HSO4, BF4, PF6), 分别用X射线能谱仪、傅里叶红外光谱、X射线衍射、扫描电镜、透射电镜、振动样品磁强计以及热重分析对其结构和理化性能进行表征, 并对油品的脱氮性能进行了研究. 结果表明: 磁性聚离子液体Fe3O4@SiO2@PILs-HSO4对模拟油品中喹啉的脱除性能最佳; 通过研究温度、时间、剂油比及循环次数等脱氮因素, 得到了最佳的脱氮条件; 在室温下当剂油比为1:10时反应30min, 模拟油品中喹啉的脱除率约为84.5%, 循环利用5次后, 脱氮效率并无明显降低, 仍表现出良好的脱氮性能; 其对真实柴油的脱氮效率达到了61.0%. 与已有报道的其他离子液体脱氮方法相比, 该方法具有成本低、操作简单、回收方便、可重复使用等优点. |
| Abstract: | Three magnetic poly(ionic liquids), Fe3O4@SiO2@PILs-X(X=HSO4, BF4, PF6), are synthesized by free polymerization of 3-acetic acid-1-vinylimidazolium bromide (VimCOOHBr) with vinyl-modified magnetic nanospheres, which is followed by anion exchange process. The structure and physical properties of synthesized magnetic nanoparticles are characterized with EDAX, FT-IR, XRD, SEM, TEM, VSM, TGA, and their denitrification performances of quinoline from the simulated oil are investigated, revealing that Fe3O4@ SiO2@PILs–HSO4 exhibits the best removal performance for quinoline. The effects of denitrification factors such as reaction time, temperature, the mass ratio of Fe3O4@SiO2@PILs–HSO4/oil, and recycle time are discussed, and the optimum denitrification conditions are obtained. The removal rate of quinoline from the simulated oil reads about 84.5% when the ratio of reagent to oil is 1:10 with 30 min of the reaction time at room temperature, and the denitrification efficiency is not obviously reduced after five cycles, in the process the denitrification efficiency of Fe3O4@SiO2@PILs-HSO4 for FCC gasoline is obtained to be around 61.0%. Compared with denitrification methods of other ionic liquids reported in literatures, the magnetic poly (ionic liquids) denitrification method in this work suggests the advantages of low cost, simple operation, convenient recycling and reusability. |
| 参考文献 /References: | [1] Anenberg S C, Miller J, Minjares R, et al. Impacts and mitigation of excess diesel-related NOx emissions in 11 major vehicle markets[J]. Nature, 2017, 545(7655):467-471. [2] Shindell D, Faluvegi G, Walsh M, et al. Climate, health, agricultural and economic impacts of tighter vehicle-emission standards[J]. Nature Climate Change, 2011, 1(1):59-66. [3] Lelieveld J, Evans J S, Fnais M, et al. The contribution of outdoor air pollution sources to premature mortality on a global scale[J]. Nature, 2015, 525(7569):367-371. [4] B?smann A, Datsevich L, Jess A, et al. Deep desulfurization of diesel fuel by extraction with ionic liquids[J]. Chemical Communications, 2001, 23:2494-2495. [5] Prajapati Y N, Verma N. Adsorptive desulfurization of diesel oil using nickel nanoparticle-doped activated carbon beads with/without carbon nanofibers: Effects of adsorbate size and adsorbent texture[J]. Fuel, 2017, 189:186-194. [6] Yang H, Chen J W, Briker Y, et al. Effect of nitrogen removal from light cycle oil on the hydrodesulphurization of dibenzothiophene, 4-methyldibenzothiophene and 4,6-dimethyldibenzothiophene[J]. Catalysis Today, 2005, 109(1/4):16-23. [7] Ding L H, Zheng Y, Zhang Z S, et al. HDS, HDN, HDA, and hydrocracking of model compounds over Mo-Ni catalysts with various acidities[J]. Applied Catalysis A: General, 2007, 319:25-37. [8] Yu H, Li S Y, Jin G Z. Catalytic hydrotreating of the diesel distillate from fushun shale oil for the production of clean fuel[J]. Energy & Fuels, 2010, 24(8):4419-4424. [9] Zhang H, Song H. Study of adsorptive denitrogenation of diesel fuel over mesoporous molecular sieves based on breakthrough curves[J]. Industrial & Engineering Chemistry Research, 2012, 51(49):16059-16065. [10] Asumana C, Yu G R, Guan Y W, et al. Extractive denitrogenation of fuel oils with dicyanamide-based ionic liquids[J]. Green Chemistry, 2011, 13(11):3300-3305. [11] Lu H, Li P, Deng C, et al. Deep catalytic oxidative desulfurization (ODS) of dibenzothiophene (DBT) with oxalate-based deep eutectic solvents (DESs)[J]. Chemical Communications, 2015, 51(53):10703-10706. [12] Lei Z, Chen B, Koo Y M, et al. Introduction: Ionic liquids[J]. Chemical Reviews, 2017, 117(10):6633-6635. [13] Hayes R, Warr G G, Atkin R. Structure and nanostructure in ionic liquids[J]. Chemical Reviews, 2015, 115(13):6357-6426. [14] Dong K, Liu X, Dong H, et al. Multiscale studies on ionic liquids[J]. Chemical Reviews, 2017, 117(10):6636-6695. [15] Vekariya R L. A review of ionic liquids: Applications towards catalytic organic transformations[J]. Journal of Molecular Liquids, 2017, 227:44-60. [16] Yamada Y M, Sarkar S M, Uozumi Y. Self-assembled poly(imidazole-palladium): Highly active, reusable catalyst at parts per million to parts per billion levels[J]. Journal of the American Chemical Society, 2012, 134(6):3190-3198. [17] Dharaskar S A, Wasewar K L, Varma M N, et al. Imidazolium ionic liquid as energy efficient solvent for desulfurization of liquid fuel[J]. Separation and Purification Technology, 2015, 155:101-109. [18] Sanghi S, Willett E, Versek C, et al. Physicochemical properties of 1,2,3-triazolium ionic liquids[J]. RSC Advances, 2012, 2(3):848-853. [19] Zhang S Z Q, Zhang Z C. Extractive desulfurization and denitrogenation of fuels using ionic liquids[J]. Industrial & Engineering Chemistry Research, 2004, 43(2):614-622. [20] Lui M Y, Cattelan L, Player L C, et al. Extractive denitrogenation of fuel oils with ionic liquids: A systematic study[J]. Energy & Fuels, 2016, 31(3):2183-2189. [21] Li J, Zeng K, Xu H, et al. Denitrification of fuel oil by hydrogen-sulfate pyrazolium-based ionic liquids[J]. Chemistry Select, 2017, 2(35):11469-11473. [22] Pourjavadi A, Hosseini S H, Doulabi M, et al. Multi-layer functionalized poly(ionic liquid) coated magnetic nanoparticles: Highly recoverable and magnetically separable br?nsted acid catalyst[J]. ACS Catalysis, 2012, 2(6):1259-1266. [23] Zheng X, He L, Duan Y, et al. Poly(ionic liquid) immobilized magnetic nanoparticles as new adsorbent for extraction and enrichment of organophosphorus pesticides from tea drinks[J]. Journal of Chromatography A, 2014, 1358:39-45. [24] 曾恺, 李杰, 季帆, 等. 吡唑型离子液体对模拟油品中吡啶的脱除性能[J]. 宁波大学学报(理工版), 2016, 29(3):93-97. [25] Nigam S, Barick K C, Bahadur D. Development of citrate-stabilized Fe3O4 nanoparticles: Conjugation and release of doxorubicin for therapeutic applications[J]. Journal of Magnetism and Magnetic Materials, 2011, 323(2):237-243. [26] Wang H, Xie C, Yu S, et al. Denitrification of simulated oil by extraction with H2PO4-based ionic liquids[J]. Chemical Engineering Journal, 2014, 237:286-290. |
| 备注/Memo: | 收稿日期: 2018-11-15. 宁波大学学报(理工版)网址: http://journallg.nbu.edu.cn/基金项目: 浙江省公益性技术应用研究计划(2015C31044).第一作者: 时运生(1993-), 男, 安徽合肥人, 在读硕士研究生, 主要研究方向: 应用化学. E-mail: 704516442@qq.com*通信作者: 张剑锋(1968-), 男, 湖南邵阳人, 教授, 主要研究方向: 材料化学. E-mail: zjf@nbu.edu.cn 宁波大学学报(理工版)网址:http://journallg.nbu.edu.cn/ |