题名 | 磁性离子液体的合成及物性研究 |
作者 | 李小华 |
学位类别 | 硕士 |
答辩日期 | 2010-05-29 |
授予单位 | 中国科学院研究生院 |
授予地点 | 北京 |
导师 | 张锁江 |
关键词 | 离子液体 磁性 数据库 物性 |
其他题名 | Study on the synthesis and physicochemical properties of magnetic ionic liquids |
学位专业 | 化学工程 |
中文摘要 | 离子液体作为新兴软功能材料,其物理和化学性质数据是相关工业设计和开发的重要基础,其性质与结构关系的研究可为新型功能化离子液体的设计开发及应用提供重要依据。磁性离子液体是带有磁性的一类离子液体,具有独特性能,它可用于反应溶剂,催化剂,分离溶剂及纳米材料制备中,特别是在工业过程中,可以避免流失所带来的物耗及能耗问题,因而,较常规离子液体而言具有更多的工程应用优势。本论文沿袭前人对离子液体数据库做了系统的工作,通过数据分析总结,合成了系列磁性离子液体,并对其物性、磁性开展了系统的研究。论文主要工作及成果如下: 1. 收集ISI数据库中2008年1月至6月文献报道的所有关于离子液体的物性数据,并整理录入Access数据库。与2007年底数据库情况比较,共增加57种阳离子、14种阴离子、144种离子液体,约300余条物性数据信息。对离子液体编号进行了相应的修改,对原本规律性不强的阴阳离子编号均变为5位数编号,前两位表示类别,后三位表示个数,不足位数的以“0”补齐,使编号更具科学性。并将数据库中纯离子液体的17000余条数据,包括每一个离子液体的名称,简称,分子量,分子式,结构,参考文献,应用以及各种物性数据,对照原文献进行了一一的校对。并整理1984至2008年6月的所有纯离子液体的物性数据,汇编成册,出版了《Ionic Liquids: Physicochemical Properties》一书。 2. 合成了十一种磁性离子液体,包括四种不同烷基链长阳离子的1-甲基-3-烷基咪唑四氯化铁[Cnmim][FeCl4](n=2,4,6,8),三种不同磁性金属络合基团阴离子的1-甲基-3-丁基咪唑四卤化铁[C4mim][FeX4](X=Br, Cl),四种不同烷基链长阳离子的双阴离子的1,1’-二甲基-3,3’-亚烷基双咪唑四氯化铁 [MIm-Cn-MIm][FeCl4]2 (n=2,4,6,8)。并对产物进行了IR、1HNMR、ESI-MS、Raman表征,验证其结构。 3. 研究了磁性离子液体的各种物理化学性质及磁性随结构及温度的变化规律。研究发现:磁性离子液体会有多个相变温度,包括熔点、玻璃化转变温度、结晶点等;温度的升高,使磁性离子液体的密度减小、粘度减小、电导率增大;阳离子侧链的增长,使磁性离子液体的熔点减小、密度减小、粘度增大、电导率减小;阴离子尺寸及相对质量的增加使磁性离子液体的密度增大、粘度增大、电导率减小;由于磁性离子液体中存在络合的金属元素,造成其阴阳离子氧化还原反应较多,电化学窗口较窄;磁性离子液体常温下为顺磁性,在低温下为铁磁性。 |
英文摘要 | Ionic liquid, as one kind of novel green medium, the physico-chemical properties are very important for both theoretical study and industrial application. Fundamental study on the Structure-Property Relationship is the basis of design and application of new ionic liquids. As a new kind of task-specific ionic liquid, magnetic ionic liquids can be used in many process such as organic synthesis, catalysis, separation, nanotechnical and so on. Because of its magnetic properties, they can be easily recycled in magnetic field, then save lots of energy, simplify the process. In this paper, ionic liquids database was standardized and more data were collected. Based on the database, a series of magnetic ionic liquids were synthesized and characterized, and the structure-property relationship was also investigated. The major work and innovative results for this dissertation are summarized as follows. 1. The physicochemical properties data of ionic liquids have been collected from public data such as publication pater, book and so on during the period from January 2008 until June 2008. 57 kinds of novel cations, 14 kinds of novel anions, 144 kinds of novel ionic liquids and nearly 300 item data were collected. Then the ID of the cations and anions were changed to five digits: the first two digits are the kinds of cations or anions, and the last three are the sequence number. 17000 data including name, abbreviation, formula, molecular weight, structure and physicochemical properties of pure ionic liquids in the database were checked with the original literatures. Based on the comprehensive physico-chemical property database, a handbook named “Ionic Liquids: Physicochemical Properties” was published. 2. Eleven magnetic ionic liquids, 1-methyl-3-alkylimidazolium tetrachloroferrate [Cnmim][FeCl4] (n=2, 4, 6, 8), 1-methyl-3-butylimidazolium tetrahalogenferrate [C4mim][FeX4](X=Br, Cl), 1,1'-dimethyl-3,3'-alkylenediimidazolium tetrachlorferrate [MIm-Cn-MIm][FeCl4]2 (n=2, 4, 6, 8) were synthesized, the structures were verified by many characterized method such as 1H-NMR, FT-IR, Raman and ESI-MS. 3. The phase transition behavior, thermal stability, density, viscosity, conductivity and magnetic susceptibility of synthesized magnetic ionic liquids were measured. The influence of the temperature and structure such as the length of the alkyl chain (R) in the cation [Cnmim], the haloid atom in the anion [FeX4] on the above properties was extensively investigated. It found that: (1) magnetic ionic liquids had multi-phase transition points, such as melting point, glass transition point, crystallization point and so on; (2) with the temperature increasing, the density and viscosity of the magnetic ionic liquid decreased while the conductivity increased; (3) with the length of the alkyl chain (R) in the cation [Cnmim] increasing, the melting point, density and conductivity of the magnetic ionic liquid decreased while the viscosity increased; (4) with the volume and molecular weight of the anion increasing, the density and viscosity of the magnetic ionic liquid increased, but the conductivity decreased; (5) since the anions of magnetic ionic liquids were metal complexes, their anions and cations had multi-redox reactions, so their electrochemical windows were not wide; (6) ionic liquids were paramagnetic at room temperature and ferromagnetic at lower temperature. |
公开日期 | 2013-09-17 |
页码 | 90 |
内容类型 | 学位论文 |
源URL | [http://ir.ipe.ac.cn/handle/122111/1521] ![]() |
专题 | 过程工程研究所_研究所(批量导入) |
推荐引用方式 GB/T 7714 | 李小华. 磁性离子液体的合成及物性研究[D]. 北京. 中国科学院研究生院. 2010. |
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