甲基羟基取代瓜环的合成、分离及超分子自组装体的研究

发布时间：2018-01-15 02:22

本文关键词：甲基羟基取代瓜环的合成、分离及超分子自组装体的研究　出处：《贵州大学》2016年硕士论文　论文类型：学位论文

【摘要】：瓜环(cucurbit[n]urils,)是一类具有疏水性空腔,且由多个苷脲通过桥联亚甲基连接起来的大环化合物,两端口修饰着羰基氧原子使其又具有配体的功能,简称Q[n]或CB[n]。自从六元瓜环(Q[6])的晶体结构被表征以来,瓜环因其独特的结构特征和潜在的应用前景,受到国内外超分子化学研究者们的广泛关注。随着瓜环合成、分离技术的不断完善,目前瓜环家族已扩展到包括普通瓜环Q[5]、Q[6]、Q[7]、Q[8]、Q[10]、tQ[14]及各种结构新颖的改性瓜环在内的近百名“成员”,在改善瓜环溶解性、提高瓜环外壁化学活性及构筑瓜环基超分子自组装体等研究领域取得了较大发展。半甲基取代瓜环是由3α-甲基取代苷脲与多聚甲醛在盐酸介质中加热回流合成得到的。半甲基取代瓜环具有十分明显的特点:1)廉价,仅次于普通瓜环,且产率最高;2)能产生聚合度大于7的瓜环体系;3)均既溶于水,又溶于有机溶剂;4)特殊的稳定性,氧化产物收率高。另外,除贵州大学的贵州省大环化学及超分子化学重点实验室外,几乎无人专门对其进行研究。因此,本论文选择半甲基取代瓜环及半羟基化半甲基取代瓜环为研究对象,在已有工作基础上,主要开展的研究内容包括:1)半羟基化半甲基取代瓜环的合成、分离提纯及结构表征;2)半羟基化半甲基取代瓜环与系列碱土金属离子、稀土金属离子的超分子自组装及其在轻重稀土分离中的探究;3)基于半甲基取代瓜环的多孔超分子自组装实体在挥发性有机分子(VOCs)的选择性吸附中的研究;4)基于半甲基取代瓜环对多种苯并咪唑类农药促溶作用的研究。基于瓜环外壁作用,以第三组分作为结构导向试剂,设计构筑瓜环超分子自组装实体已成为瓜环化学的一个新研究方向。本论文基于上述理论成功构筑一系列瓜环基超分子自组装体,并在VOCs的吸附、系列稀土金属离子的识别及分离、农药分子的促溶等方向取得一定进展,有效拓展了改性瓜环在超分子化学领域的研究范围。
[Abstract]:Cucurbit. [N] urilsn) is a class of macrocyclic compounds with hydrophobic cavities connected by a plurality of glycosides via bridged methylene, with two-port modification of carbonyl oxygen atoms to make them have the function of ligands. [N] or CB. [Since the six yuan melon ring Q. [6) since its crystal structure was characterized, melons have attracted wide attention from supramolecular chemistry researchers at home and abroad for their unique structural characteristics and potential application prospects. With the continuous improvement of separation technology, the current melon ring family has been extended to include ordinary melon ring Q. [5] ,Q. [6] ,Q. [7] ,Q. [8] ,Q. [10] ,tQ. [14] and various novel structures of modified melon rings include nearly 100 "members" in improving the solubility of melon rings. Great progress has been made in improving the chemical activity of the outer wall of melons and in constructing supramolecular self-assembled melons. Semi-methyl substituted melons are refluxed by heating 3 伪 -methyl-substituted glucuronide and paraformaldehyde in hydrochloric acid medium. The semi-methyl substituted melons have very obvious characteristics:. 1). Cheap. Second only to the common melon ring, and the highest yield; 2) the melons with polymerization degree greater than 7 can be produced; 3) both soluble in water and in organic solvents; 4) special stability and high yield of oxidized products. In addition, except for the key laboratory of macrocyclic chemistry and supramolecular chemistry of Guizhou University, almost no one has studied it specially. In this paper, we choose semi-methyl substituted melon ring and semi-hydroxylated semi-methyl substituted melon ring as the research object. Based on the previous work, the main research contents include the synthesis of semi-hydroxylated semi-methyl substituted melon ring. Separation, purification and structure characterization; 2) the supramolecular self-assembly of semi-hydroxylated semi-methyl substituted melons and a series of alkali earth metal ions, rare earth metal ions and their application in the separation of light and heavy rare earths; 3) selective adsorption of volatile organic molecules (VOCs) by porous supramolecular self-assembled entities based on semi-methyl substituted melons; 4) based on the study on the solubilization of benzimidazole pesticides by semi-methyl substituted melons, the third component was used as the structure-oriented reagent based on the outer wall of the ring. The design and construction of supramolecular self-assembly entities has become a new research direction of ring chemistry. Based on the above theory, a series of supramolecular self-assembled melons have been successfully constructed and adsorbed on VOCs. Some progress has been made in the recognition and separation of rare earth metal ions and the promotion of solubilization of pesticide molecules, which has effectively expanded the research scope of modified melon rings in the field of supramolecular chemistry.
【学位授予单位】：贵州大学
【学位级别】：硕士
【学位授予年份】：2016
【分类号】：O641.3

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