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Molecular architecture of inorganic complex multilayers based on surface coordination chemistry

基于表面配位化学的无机复合多层膜的分子结构

基本信息

批准号：
09440233
负责人：
HAGA Masa-aki
金额：
$ 7.49万
依托单位：
CHUO UNIVERSITY (1998)Okazaki National Research Institutes (1997)
依托单位国家：
日本
项目类别：
Grant-in-Aid for Scientific Research (B)
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

The design and fabrication of meso molecular structures on the surface is one of the important and attractive areas in the future material science. In order to construct the meso molecular structures in two dimensions, we employed two methodologies for molecular fabrication on the surface ; one is the self-assembled monolayer (SAM) method on gold, and the other is Langmuir-Blodgett (LB) technique, in both of which coordination bond is used for a chemical "glue" between the molecular module. New anchoring or amphiphilic ligands based on tridentate 2,6-bis(benzimidazol-2-yl)pyridine(L18) and their Ru complexes, [Ru(L18)(X)]^<n+>(X = tridentate or tins monodentate ligand) were synthesized and used as a molecular building block. At the air-water interface, surface pressure-area (pi-A) isotherms showed strong dependence on the subphase condition such as pH or metal ion (Zn^<2+>, Cd^<2+> and Mn^<2+>) for Ru complex containing 2,2' : 6", 2'-terpyridine-4-phosphonate(X= tpy-PO_3H). The surface morphology of the transferred LB films on mica substrates, which was obtained from an AFM image, revealed a relatively regular stripe structure. The surface morphology was also dependent on the auxiliary ligand X.In the case of X = 2,3,5,6-tetrakis(2'-pyridyl)pyrazine, a circular domain structure was observed.Furthermore, the molecular orientation of the Ru complex molecules at the air-water interface was proved by the intensity of MLCT band around 500 nm in in-situ UV spectral measurements. We found that the intensity of MLCT band around 500 nm was changed by pH change or metal coordination from the subphase.

表面介观分子结构的设计与制备是未来材料科学的重要研究方向之一。为了构建二维的介观分子结构，我们采用了两种表面分子制造方法：一种是在金上的自组装单层（SAM）方法，另一种是LB技术，在这两种方法中，配位键被用作分子模块之间的化学“胶水”。合成了一种新的基于2，6-二（苯并咪唑-2-基）吡啶（L18）的锚定或两亲配体及其钌配合物[Ru（L18）（X）]^<n+>（X =三齿或单齿配体），并将其用作分子结构单元.在空气-水界面上，含2，2 '：6'，2 '-三吡啶-4-膦酸酯（X= tpy-PO_3 H）的钌配合物的表面压力-面积（pi-A）等温线显示出对亚相条件如pH或金属离子（Zn^<2+>、Cd^<2+>和Mn^<2+>）的强烈依赖性。从AFM图像中得到的转移到云母衬底上的LB膜的表面形貌显示出相对规则的条纹结构。当X = 2，3，5，6-四（2 '-吡啶基）吡嗪时，Ru配合物分子在空气-水界面上形成了环状畴结构，并通过原位紫外光谱中500 nm附近的MLCT谱带强度证实了Ru配合物分子在空气-水界面上的分子取向.我们发现，MLCT带附近的500 nm的强度被改变的pH值的变化或金属配位从亚相。