Development of Interfaces with Signal Transaction Ability and Its Application to Molecular Sensing

根据项目计划，我们开展了以下三个项目：（1）开发能够选择性客体结合的复杂主体化合物，其中可以通过容易观察到的信号来告知，（2）制造能够进行分子识别和信号转导的有机薄膜，（3）设计和开发易于制造并显示出优异分子识别能力的“二维分子印迹”薄膜。关于项目（1），我们已经开发了几种新的具有富电子或缺电子侧基的环糊精基主体。将侧基共价连接到环糊精上，不仅提高了分子识别能力，而且实现了良好的信号转导。在所开发的主体中，发现芘附加的环糊精是联吡啶和一些卤代化合物的优良主体，这些化合物被称为环境污染物。我们还有合成人 ...更多信息 研究了几种环糊精衍生物与冠醚或铵化合物的偶联，发现它们具有不同的分子识别能力，并且发现偶联概念可以用于构建复杂的主体化合物，即使在水溶液中也是如此。关于项目（2），我们已经成功地制备了几种由改性环糊精、聚电解质或两者组成的有机薄膜。此外，我们还发现偶氮苯修饰的聚电解质的分子识别能力可以通过偶氮基团的光异构化来控制，并且可以通过环糊精络合来组装均匀带电的聚电解质。此外，修饰的环糊精单分子膜被发现是一种薄膜，能够区分分析物的电荷状态。关于项目（3），我们探讨了几种方法，实现“二维分子印迹”的方法，利用环糊精，cnwether，和正或负电荷的烷烃的自组装技术。不幸的是，我们还没有获得具有良好质量和分子识别性能的混合单分子膜。必须作出进一步努力，|提升这个概念。少

According to the project plan, we have conducted following three projects; (1) development of the sophisticated host compounds capable of selective guest binding for which one could be informed by readily observable signals, (2) fabrication of organic thin films capable of molecular recognition and signal transduction, and (3) designing and development of "two-dimensional molecular imprinting" thin films that would be easily fabricated and would show excellent molecular recognition ability.Regarding the project (1), we have developed several novel cyclodextrin-based hosts possessing electron-rich or electron-deficient pendant residue. The pendants were covalentiy attached to cyclodextrin for not only improving the molecular recognition ability but also realizing excellent signal transduction. Of the hosts developed, pyrene-appended cyclodextrins were found as excellent hosts for bipyridinium and some halogenated compounds, which are known as environmental pollutants. We have also synth … More esized several cyclodextrin derivatives coupled with crownether or ammonium compound that exhibited different abilities on molecular recognition, and have found that the coupling concept was usable in constructing sophisticated host compounds even in aqueous solution.Regarding the project (2), we have successfully fabricated several organic thin films consisting of modified cyclodextrins, polyelectrolytes, or both. In addition, we have found that the molecular recognition ability of azobenzene-modified polyelecrolytes could be controlled by photo-isomerization of the azo groups, and that uniformly charged polyeletrolytes could be assembled by cyclodextrin complexation. Moreover, monolayers consisting of modified cyclodextrins were found to be thin film capable of discriminating charging state of the analytes.Regarding the projext (3), we have approached several ways to realize the "two-dimensional molecular imprinting" methodology by use of cyclodextrin, cnwnether, and positively or negatively charged alkanes based on the self-assembled technique. Unfortunately, we have not obtained mixed monolayers with good quality and molecular recognition properties. Further efforts must be required for |leveloping this concept. Less