含卟啉和C60的铁铁氢化酶模型物的设计合成及催化功能研究

This project is to study the synthesis, structure, propertiy, and particularly the catalytic H2-producing function of the [FeFe]-hydrogenase active site model complexes containing porphyrin and C60 moieties. The main purpose of this study is to develop organometallic reactions and synthetic methods, and to synthesize a new generation of [FeFe]-hydrogenase active site model compounds with unique structure and novel properties. In addition, through systematic study on the synthesis, structural and catalytic function of the target model complexes, it will allow us to be able to select one or two artificial H2-producing catalysts with superior catalytic activity and to find the relationship between their structures and catalytic function. This project is of theoretical and practical interest and it will greatly promote development of organometallic chemistry, biomimetic chemistry and the other closely related areas such as catalysis, energy source and material science.

本项目旨在研究既含卟啉环又含富勒烯C60的氢化酶活性中心模型物三元组装体的合成、结构、性质及催化还原质子为氢气的功能。通过本项目系统深入的研究，发展金属有机合成方法学和金属有机化合物反应化学并合成一系列结构和性质新颖的新一代铁铁氢化酶活性中心模型物。本项目将在前体和目标模型物的合成及结构表征的基础上系统研究它们催化质子还原为氢气的能力，优选1-2种催化功能良好的产氢催化剂并总结结构与功能的关系及规律。本项目研究对促进金属有机化学、生物酶仿生化学、催化及能源材料等多种学科的发展，具有重要理论和实际意义。

本项目设计合成了一系含光敏剂卟啉或C60二元组装体的铁铁氢化酶模型物，以及既含卟啉又含C60的三元组装体的铁铁氢化酶模型物，用各种现代物理化学方法充分表征了它们的结构，发现了合成这类结构新颖模型物的某些简便的合成方法，研究了其中某些模型物的电化学性质及催化质子还原为氢气的功能。本项目研究成果对促进铁铁氢化酶仿生化学的发展具有重要理论意义和潜在的应用价值。

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