水解酶催化多组分多米诺反应合成螺环化合物方法及其催化机理

开展结构复杂、具有重要应用功能的螺环化合物的新合成方法学研究具有重要科学意义和应用前景。本项目利用一种酶能催化多种反应的性质，设计脂肪酶催化的多组分反应体系，实现了螺恶嗪类化合物的一锅法合成；我们对该新方法中酶催化剂的类别、反应介质、酰胺种类、温度、底物结构等反应参数对反应的影响规律加以研究，通过底物结构的设计来实现具有不同骨架结构、取代结构的螺环化合物的构筑；进一步探讨该酶促多组分反应的内在本质和酶的催化作用，提出相应机理模型，并设计实验加以验证；在此基础上，通过考察这类含氮、氧杂螺环化合物的荧光、光致变色等光学性质，认识这类螺环化合物的结构与其光学性质间的关系，探讨其在光学材料方面可能的应用价值。本项目将有助于推动生物催化多组分反应的发展，认识酶催化多功能性的本质，建立的脂肪酶催化一锅法合成螺恶嗪类化合物的新方法能在螺环类光学材料合成中得到重要应用。

It is very important to develop new synthesis methodologies for spirocompounds with complicated structures and wide applications. This project designed lipase-catalyzed multicomponents reaction based on enzymatic promiscuity, successfully achieved one-pot synthesis of Spirooxazino derivatives. We investigated the effect of enzyme sources, reaction media, temperature, and substrate structures etc. on the lipase-catalyzed MCRs. A series of spirocompounds with different skeleton and substitutions can be efficiently prepared. The mechanism and pathway for the lipase-catalyzed MCRs will be discussed and confirmed by some designed experiments. Furthermore, the project will investigate the photo-physical property of synthesized spirocompounds and demonstrate the potent application. Results of this project will be helpful for the development of biocatalytic MCRs, and expand the wide application of spirocompounds into organic optoelectronics materials.