Creation of Self-Organized Fullerene-Lipid Chemistry

本研究在设计合成富勒烯-脂质杂化材料和富勒烯-脂质复合材料的基础上，建立了“自组织富勒烯化学”。所得结果总结如下1。合成了一种携带C_<60>-的水溶性单链两亲铵类化合物10-（n -甲基-2- fulleroprrolidyl）十二烷基三甲基溴化铵(1)。化合物1在水溶液中通过1的自组织产生10-12层厚度的纤维状聚集体和盘状聚集体。x射线衍射研究表明，1的铸膜形成多层结构。对水溶液和在电极上的1单独和1加入脂质膜的铸膜的电化学反应表明，在电极上的1单独和1/脂质膜发生电子转移反应，导致富勒烯阴离子或三阴离子的生成。该研究为构建基于自组装分子组织的更有序结构的电活性富勒烯纳米结构提供了可能性。高富勒烯C_<84>嵌入电极上的分子双层阳离子脂质铸膜中，发生明显的电子转移反应，生成C_<84>多电荷阴离子。这一结果在富勒烯的化学和物理方面具有基础意义和应用意义。采用核磁共振、紫外、红外光谱、差示扫描量热法（DSQ）、x射线衍射和电化学等多种技术表征了含C_<60>、C_<16>、C_<14>和C_<12>三烷基链的人工脂的独特性质。研究了脂质膜的相变过程。在富勒烯脂修饰的电极装置上调节电化学是可能的。富勒烯脂质中电生成的单阴离子和双阴离子与大尺寸的四正丁基铵离子和四正丁基膦离子的“软”电解质阳离子结合较强，本研究为构建富勒烯脂质双分子层器件提供了指导，为富勒烯的纳米科学和纳米技术研究提供了依据。少

This study has been carried out to establish "self-organized fullerene chemistry" based on the design and syntheses of fullerene-lipidit hybrid and fullerene-lipid composite materials. The obtained results are summarized below.1. A water-soluble C_<60>-carrying single-chain ammonium amphiphile, 10-(N-Methyl-2-fulleropyrrolidyl) decyltrimethylammonium bromide (1) was synthesized. Compound 1 produces both fibrous aggregates and disk-like aggregates with 10-12 run of thickness through self-organization of 1 in aqueous solution. X-ray diffraction study suggests that cast films of 1 form a multi-layer structure. Electrochemistry for an aqueous solution and for cast films of 1 solely and 1 incorporated in lipid films on electrodes revealed that films of 1 solely and of 1/lipid cast on electrodes showed electron transfer reactions leading to the generation of the fullerene dianion or trianion. The study opens possibilities for the construction of electroactive fullerene-nanoarchitectures with … More ordered structure based on self-assembled molecular organization.2. The higher fullerene C_<84> embedded in cast films of molecular-bilayer-forming cationic lipids on electrodes was found to exhibit evident electron transfer reactions leading to the generation of C_<84> multi-charged anions. This result has both fundamental and applied implications in the chemistry and physics of fulerenes.3. The Unique properties of C_<60>-bearing artificial lipids with a triple-alkyl chain of C_<16> , C_<14>, or C_<12> were characterized by a variety of techniques including ^<13>C NMR, UV-vids and FT-IR spectroscopies, differential scanning calorimetry (DSQ, X-ray diffraction, and electrochemistry. The phase transitions of the lipid films were presented. Regulated electrochemistry at the fullerene lipid-modified electrode devices was possible. The electrogenerated radical monoanions and dianions of the fullerene lipids were found to bind strongly with "soft" electrolyte cations with large size tetra-n-butylammonium and tetra-n-butylphosphonium ions, the present study guides us toward construction of fullerene lipid bilayer devices which might be useful in the field of nanoscience and nanotechnology of fullerenes. Less