Development of environment-conscious synthetic reactions : construction of reaction coordinate-response catalyst

节约环境和资源是人类面临的最紧迫的问题。为了解决这一问题，构建一个可持续发展的社会，开发选择性、原子效率高和环境友好的合成反应是必不可少的。生物材料转化系统具有高选择性、原子效率高、绿色环保等优点，但目前大多数生物材料转化系统中都有几种酶参与，而目前的化学方法很难实现。为了在催化剂的作用下实现同样绿色高效的反应，我们设计了可以改变其结构并沿反应坐标表现出适当催化性能的络合物。以这种配合物为催化剂，以分子氧或过氧化氢为末端氧化剂，可成功地实现高对映选择性和原子效率高的氧化反应。本研究证明了一种催化剂可以沿反应坐标改变其催化性能，从而实现绿色反应的有效性。

Environment and resource conservation is the most urgent issue that human beings face. To address this issue and construct a sustainable society, development of selective, atom-efficient and eco-friendly synthetic reactions is essential. Biological material transformation systems are highly selective and atom-efficient and green, but several enzymes participate in most biological systems that are difficult to be implemented by the current chemical way. To realize equally green and efficient reactions with a catalyst, we designed complexes that can change their structure and exhibit an appropriate catalytic performance along reaction coordinate. With such complexes as catalyst, we could successfully achieve highly enantioselective and atom-efficient oxidation reactions using molecular oxygen or hydrogen peroxide as the terminal oxidant. This research demonstrated the effectiveness of a catalyst that can change its catalytic performance along reaction coordinate, for realizing a green reaction.