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Organic Synthesis of Transition Metal Encapsulated Fullerenes

过渡金属封装富勒烯的有机合成

基本信息

批准号：
09650960
负责人：
TOBE Yoshito
金额：
$ 2.18万
依托单位：
Osaka University
依托单位国家：
日本
项目类别：
Grant-in-Aid for Scientific Research (C)
财政年份：
1997
资助国家：
日本
起止时间：
1997 至 1998
项目状态：
已结题

项目摘要

1. Spectroscopic Studies on the Structures of Cyclocarbons : Molecular structures of cyclo[n]carbons (n= 12, 16, 18, 20, and 24), which were generated in the laser-desorption mass spectroscopic method from the corresponding organic precursors, were investigated on the basis of the ultraviolet photoelectron spectra of the cluster anions.It was revealed that the cyclo[n]carbons with 4n carbons possess polyynes structure whereas those with 4n+2 carbons are cumulenic structure.2. Generation of Cage Polyyne (C_<60>H_6) and its Isomerization into Fullerene : A precursor to the cage polyyne C_<60>H_6 was prepared in order to investigate the possibility regarding dehydrogenative isomerization of C_<60>H_6 into C_<60> fullerene.In the laser-desorption mass spectra of the precursor, we observed not only C_<60>H_6 derived from elimination of six indane molecules but also C_<60> fullerene which was formed presumably by the isomerization of the reactive polyyne chain.These results suggest the possible total synthetic pathway of fullerenes and their metal encapsulated derivatives on the basis of polyyne cyclization.3. Generation of Cage Azapolyyne (C_<58>N_2H_4) and its Isomerization into Diazafullerene : The cage polyyne C_<58>N_2H_4 having two pyridine rings was generated from the corresponding organic precursor by the same method as described above.In the laser-desorption mass spectra, we observed not only C_<58>N_2H_4 but also a small peak due to diazafullerene C_<58>N_2.This is an important finding with regard to the synthesis of metal encapsulated fullerenes, because it represents the first observation of this novel heterofullerene which is isoelectronic with fullerene dianion.

1.环碳化合物结构的光谱研究：环[n]碳的分子结构（n= 12、16、18、20和24），它们是在激光解吸质谱法中由相应的有机前体产生的，通过紫外光电子能谱研究了簇合物阴离子的结构，发现环[n]含4n个碳原子的碳原子具有多炔结构，而含4n+2个碳原子的碳原子具有累积多炔结构.笼状多炔（C_ H_6）的生成<60>及其异构化为富勒烯：为了研究笼状多炔C_<60>H_6的异构化为富勒烯的可能性，我们制备了笼状多炔C_ H_6<60>的前体<60>，在前体的激光解吸质谱中，我们观察到了<60>由六个茚满分子的消除生成的C_ H_6和<60>可能由反应性多炔链的异构化生成的富勒烯，这些结果提示了富勒烯及其金属包封衍生物的可能的基于多炔环化的全合成途径.笼状氮杂多炔（C_ N_2H_4）的生成<58>及其异构化为二氮富勒烯：<58>用同样的方法从相应的有机前体中生成了具有两个吡啶环的笼状多炔C_ N_2H_4。在激光解吸质谱中，我们不仅观察到C_<58>N_2H_4，而且还观察到一个由二氮富勒烯C_N_2引起的小峰<58>。这是金属包裹富勒烯合成中的一个重要发现，因为它代表了这种与富勒烯二价阴离子等电子的新型杂富勒烯的首次观察。