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Research on Combinatorial Functions of Integrated Organic Redox Systems and their Applications for Unimolecular Memory

集成有机氧化还原系统的组合功能及其在单分子存储中的应用研究

基本信息

批准号：
15350019
负责人：
SUZUKI Takanori
金额：
$ 8.58万
依托单位：
Hokkaido University
依托单位国家：
日本
项目类别：
Grant-in-Aid for Scientific Research (B)
财政年份：
2003
资助国家：
日本
起止时间：
2003 至 2005
项目状态：
已结题

项目摘要

This project has been planned to develop new design concepts on the novel organic responding molecules based on the integration of redox active molecules. The major themes to be tackled with are as follows : (1) Redox response systems with electrochemical bistability and surface modifying properties ; (2) New synthetic strategy for the fused- polyether structures ; (3) Redox active molecules with phase transition properties triggered by external stimuli.We have succeeded in preparing redox systems to meet the requirement in the first theme, and some of them are further endowed with multi-input and multi-output fuctionalities. The disuflide unit or ethynyl groups were selected that act as surface-binding linkers for Au an Si, respectively. Preparation of SAM and examination toward the realization of unimolecular memory are now under way.The fused-polyether skeleton found in some marine natural products should be a suitable motif for studying the aggregation by weak C-H--O hydrogen bonds … More . In the second theme, facile and general convergent strategy was developed for a variety of polyether skeleton. Based on the newly developed protocol based on the reaction between an aldehyde and an acylanion equivalent, we could synthesize polyetheral natural product (hemibrevetoxin B) and the large segments of ciguatoxins with 4-5 ether units. X-ray analyses on some of them have revealed that several short C-H--O contacts were observed that connect tape-shaped polyethers tol the stacked or dimeric strucures. Not only natural but also non-natural polyethers are shown worth investigated.Reversible oligomerization of bis(diarylethenyl)arenes-type electron donors upon oxidation is the outstanding achievement in terms of the third theme. Deeply-colored polycation oligomers could be isolated as stable salts that regenerated the starting monomeric donors upon reduction. By attaching long alkyl chains on the aryl groups, some of these materials act as organic gelators, thus giving a new desing concept for the dynamic mesophase, whose properties can be modulated by electrochemical input. Less

本项目旨在开发基于氧化还原活性分子整合的新型有机响应分子的新设计概念。主要研究内容包括：（1）具有电化学双稳性和表面改性性能的氧化还原反应体系：（2）新的稠合聚醚结构合成策略;（3）具有相变性质的氧化还原活性分子，我们成功地制备了满足第一个主题要求的氧化还原体系，有的还被赋予了多输入多输出的功能。选择二硫醚单元或乙炔基分别作为Au和Si的表面结合接头。SAM的制备和实现单分子记忆的研究正在进行中，一些海洋天然产物中的稠合聚醚骨架是研究弱C-H-O氢键聚集的合适基元 ...更多信息 .在第二个主题中，我们发展了一种简便而通用的聚合策略，适用于各种聚醚骨架。基于醛与酰基阴离子等价物反应的新方法，我们可以合成聚醚醛天然产物（半短尾蛇毒素B）和具有4 - 5个醚单元的大片段雪卡毒素。X射线衍射分析表明，在聚醚的叠层或二聚体结构中，存在着若干个短的C-H-O接触。在第三个主题中，双（二芳基乙烯基）芳烃类电子给体的可逆氧化齐聚反应是研究的突出成果。深色聚阳离子低聚物可以分离为稳定的盐，还原后再生的起始单体供体。通过在芳基上连接长的烷基链，这些材料中的一些充当有机胶凝剂，从而为动态中间相提供了一种新的设计概念，其性质可以通过电化学输入来调节。少

项目成果

期刊论文数量（27）

专著数量（0）

科研奖励数量（0）

会议论文数量（0）

专利数量（0）

Isolation and Low-temperature X-ray Analysis of Intramolecular Triarylmethane-Triarylmethylium Complex : Preference of C-H Bridged Unsymmetric Structure Exhibiting Facile 1,5-Hydride Shift and Charge-Transfer interaction

分子内三芳基甲烷-三芳基甲基络合物的分离和低温 X 射线分析：优先选择 C-H 桥联不对称结构，表现出轻松的 1,5-氢化物位移和电荷转移相互作用

DOI：
发表时间：
2005
期刊：
J.Am.Chem.Soc. 127(35)
影响因子：
0
作者：
T. Suzuki;他;T.Suzuki;T.Suzuki;T.Suzuki;T.Suzuki;T.Suzuki;R.Katoono;R.Katoono;H.Kawai
通讯作者：
H.Kawai

Stereospecific Change in Conformation upon Complexation of an Exoditopic Tetraamide Host with a Bis(ammonium) Guest : Chiral Recognition and Strong CD Signaling

异位四酰胺主体与双（铵）客体络合后构象的立体特异性变化：手性识别和强 CD 信号传导

DOI：
发表时间：
2005
期刊：
Chem.Commun. (41)
影响因子：
0
作者：
T. Suzuki;他;T.Suzuki;T.Suzuki;T.Suzuki;T.Suzuki;T.Suzuki;R.Katoono;R.Katoono;H.Kawai;H.Kawai;H.Kawai;T.Suzuki;R.Katoono
通讯作者：
R.Katoono

T.Suzuki, T.Nagasu, H.Kawai, K.Fujiwara, T.Tsuji: "Formation of Keto-carbeniums from 1,2,2-Triarylacenaphthen-1-ols by Breaking a Long C-C bond : Unusual Alcohol Protonolysis Accompanied by Formal Hydride Abstraction"Tetrahedron Lett.. 44. 6095-6098 (2003

T.Suzuki、T.Nagasu、H.Kawai、K.Fujiwara、T.Tsuji：“通过破坏长 C-C 键从 1,2,2-三芳基苊-1-醇形成酮碳鎓：不寻常的醇质子分解伴随