用于催化不对称转移化的化聚合物二联体
Yaodong Lin1, Guangqing Xu1, Wenjun Tang1,2
1State Key Laboratory of Chemical Biology, Shanghai Institute of Organic Chemistry, University of Chinese Academy of Sciences, 345 Ling Ling Road, Shanghai 200032, China.
新的聚合物性胺配体形成了不对称转移化的高效催化剂. 这些可回收的催化剂产生具有高反选择性和循环数量的光学活性醇,为合成有价值的化合物提供实用解决方案.
科学领域:
- 有机金属化学
- 不对称的催化
- 聚合物化学
背景情况:
- 不对称转移化 (ATH) 对于合成性分子至关重要.
- 开发高效,可回收和高度选择性的催化剂仍然是一个关键挑战.
- 聚合联体在催化剂稳定性和可回收性方面具有潜在的优势.
研究的目的:
- 开发用于不对称催化剂的新型聚合物化胺连接体.
- 研究它们在ATH中的复合物的催化性能.
- 探索连接体结构和催化效率之间的关系.
主要方法:
- 通过二博模拟不对称的还原性合物合成聚合物性二胺联体.
- 与合成的配体形成复合物 (Ir-多胺).
- 在功能化的不对称转移化中使用Ir-多胺催化剂.
主要成果:
- 聚胺催化剂在ATH中表现出高效率和可回收性.
- 对于光学活性二次醇,获得了优异的反选择性 (高达99% ee).
- 在六个周期中,总营业额 () 达到了12000多,这是前所未有的.
- 较长的聚合物链与更高的催化反应性相关.
- 一个可信的禁用机制被提出.
结论:
- 聚合奇拉二胺使得高度活性和可回收的ATH催化剂的开发成为可能.
- 聚胺系统为高效的酶选择性合成提供了一个强大的平台.
- 这种方法为维生素B5和等重要化合物的ATH提供了实际解决方案.
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