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Development of Artificial Enzymes by Surface Molecular Imprinting

通过表面分子印迹开发人工酶

基本信息

批准号：
12450335
负责人：
FURUSAKI Shintaro
金额：
$ 8.38万
依托单位：
Sojo University (2001)Kyushu University (2000)
依托单位国家：
日本
项目类别：
Grant-in-Aid for Scientific Research (B)
财政年份：
2000
资助国家：
日本
起止时间：
2000 至 2001
项目状态：
已结题

项目摘要

A molecular imprinting technique is one of the promising approaches to design "tailor-made" catalytic sites. However, it still has two fundamental drawbacks : difficulties to introduce water-soluble substrates as an imprinting molecule in the catalytic sites, and slow catalytic kinetics arising from the inner diffusion of substrates toward the catalytic sites formed deeply in the polymer matrix. To conquer these problems, we proposed a novel molecular imprinting technique for constructing recognition sites on the polymer surface called "surface molecular imprinting technique". An imprinted polymer was prepared by polymerizing water-in-oil (W/0) emulsions containing a functional host molecule, an imprint molecule and a cross-linking agent.In this study, we designed a novel functional host molecule possessing a high inter facial activity, considering that the host molecule should be located at water-oil interface to yield a high specific recognition. Furthermore we introduced an imidazole molecule as a functional group to catalyze the hydrolysis reaction of substrates. Using the newly synthesized functional host molecule, an enzyme-mimic polymer was prepared by imprinting a substrate analogue through the complex formation between a cobalt ion and the imidazole moiety. The catalytic properties of artificial biocatalysts were investigated on the hydrolysis reaction of an amino acid ester by comparing to control experiments. The enzyme-mimic biocatalyst showed a high activity and maintained high stability for a long time.

分子印迹技术是一种很有前途的设计“定制”催化位点的方法。然而，它仍然有两个基本的缺点：难以引入水溶性基板作为印迹分子在催化位点，和缓慢的催化动力学所产生的内部扩散的基板向催化位点形成的聚合物基质中。为了克服这些问题，我们提出了一种在聚合物表面构建识别位点的新型分子印迹技术--表面分子印迹技术。采用油包水乳液聚合法制备了一种印迹聚合物，该聚合物中含有功能主体分子、印迹分子和交联剂，考虑到主体分子必须位于水-油界面，才能产生高的特异性识别，设计了一种具有高界面活性的功能主体分子。此外，我们引入了咪唑分子作为功能基团来催化底物的水解反应。使用新合成的功能性主体分子，通过钴离子和咪唑部分之间的络合物形成的底物类似物的印迹制备酶模拟聚合物。以氨基酸酯水解反应为研究对象，考察了人工生物催化剂的催化性能。该模拟酶生物催化剂具有较高的催化活性和较长时间的稳定性。