State Key Laboratory for Oxo Synthesis and Selective Oxidation, Suzhou Research Institute of LICP, Lanzhou Institute of Chemical Physics (LICP), Chinese Academy of Sciences (CAS), Lanzhou, 730000, P.R. China.
University of Chinese Academy of Sciences, Beijing, 100049, P.R. China.
Angew Chem Int Ed Engl. 2017 Jan 19;56(4):1077-1081. doi: 10.1002/anie.201610473. Epub 2016 Dec 30.
A highly enantioselective regiodivergent addition of alkoxyallenes to pyrazolones was developed to afford multiply functionalized alkylated products bearing a quaternary carbon stereocenter in high yields with excellent stereoselectivities. One approach is enabled by palladium catalysis, thus leading to branched allylic pyrazol-5-ones under mild reaction conditions. The other is catalyzed by a chiral Brønsted acid to give linear products exclusively. Moreover, the usefulness of this new method was highlighted by converting the allylic products into other interesting multifunctionalized pyrazolone derivatives which would be of great potential for the exploitation of pharmaceutically important molecules.
发展了一种高对映选择性的区域发散性的烷氧基丙二烯与吡唑酮的加成反应,以高产率和优异的立体选择性得到带有季碳原子手性中心的多官能化烷基化产物。一种方法是通过钯催化实现的,因此在温和的反应条件下得到支链烯丙基吡唑-5-酮。另一种方法则是由手性布朗斯台德酸催化得到的,只得到线性产物。此外,通过将烯丙基产物转化为其他有趣的多功能化吡唑啉酮衍生物,这种新方法的实用性得到了突出,这些衍生物对于开发具有重要药用价值的分子具有巨大的潜力。