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Studies on a luminescent reaction mechanism of ion-sensing bio-and chemiluminescence systems

离子传感生物和化学发光系统的发光反应机理研究

基本信息

批准号：
11640578
负责人：
HIRANO Takashi
金额：
$ 2.11万
依托单位：
The University of Electro-Communications
依托单位国家：
日本
项目类别：
Grant-in-Aid for Scientific Research (C)
财政年份：
1999
资助国家：
日本
起止时间：
1999 至 2000
项目状态：
已结题

项目摘要

This research project aims to establish the bioluminescence mechanism of the photoprotein aequorin(AQ)which has a calcium-ion sensing, efficient luminescence, and color-regulation properties, and to make a fundamental theory for molecular design of desirable chemiluminescent molecules. Structure elucidation of coelenteramide during AQ bioluminescence is an important problem in the bioluminescence mechanism. To clarify this problem, the fluorescent properties of the phenolate anions of coelenteramide analogues were investigated. Fluorescence of phenolate anion in non-polar solvents was observed by electronic excitation of a hydrogen-bonded complex of a coelenteramide analogue with a hydrogen-bond donor molecule. In polar solvents, phenolate anion was directly generated by using a base, and its fluorescence was studied. The se results confirm that the singlet-excited stated of phenolate anion of coelenteramide has an intramolecular CT character. The fluoro substituent effect on the fluorescent property of phenolate anions was also clarified and explained the bioluminescent pr operty of the fluorinated semi-synthetic AQ.These results consistenly support the assignment that phenolate anion is the ionic structure of the excited light-emitter in BFP during AQ bioluminescence.To establish the molecular mechanism of the lumi nescence reaction of the substrate(an imidazopyrazinone derivative)of AQ bioluminescence, we have investigated fundamental physical properties of imidazopyrazinone derivatives and their electron transfer reactivity, and found an inter molecular addition reactivity with electron-acceptor molecules. We also found that an imidazopyrazinone derivative acted as a ligand for making metal complexes. To confirm these new findings, detailed studies on the physical property and reactivity of imidazopyrazinone derivatives are in progress.

本研究项目旨在建立具有钙离子传感、高效发光和颜色调节特性的光蛋白水母发光蛋白（AQ）的生物发光机制，并为理想化学发光分子的分子设计奠定基础理论。 AQ生物发光过程中腔肠酰胺的结构解析是生物发光机制中的一个重要问题。为了澄清这个问题，研究了腔肠酰胺类似物的酚阴离子的荧光特性。通过电子激发腔肠酰胺类似物与氢键供体分子的氢键复合物，观察到非极性溶剂中苯酚阴离子的荧光。在极性溶剂中，使用碱直接产生酚阴离子，并研究其荧光。这些结果证实了腔肠酰胺酚阴离子的单重态激发态具有分子内CT特征。阐明了氟取代基对酚根阴离子荧光性质的影响，解释了含氟半合成AQ的生物发光特性。这些结果一致支持了酚根阴离子是AQ生物发光过程中BFP中激发发光体的离子结构这一假设。咪唑并吡嗪酮衍生物）的AQ生物发光，我们研究了咪唑并吡嗪酮衍生物的基本物理性质及其电子转移反应性，发现了与电子受体分子的分子间加成反应性。我们还发现咪唑并吡嗪酮衍生物可作为制备金属配合物的配体。为了证实这些新发现，对咪唑并吡嗪酮衍生物的物理性质和反应性的详细研究正在进行中。