Department of Chemistry, University of Texas at Austin, Austin, Texas 78712, United States.
J Am Chem Soc. 2022 Jan 19;144(2):1016-1022. doi: 10.1021/jacs.1c12063. Epub 2022 Jan 10.
The total synthesis of soraphen A, a myxobacterial metabolite and inhibitor of acetyl CoA carboxylase, was completed in 11 steps (longest linear sequence), less than half the steps previously required. Seven metal-catalyzed processes were deployed to unlock step-economy (comprising five asymmetric processes and four C-C bond formations). The present route does not utilize chiral auxiliaries, and four of five C-C bond formations exploit non-premetalated partners. To maximize convergency, an asymmetric Tsuji reduction was developed using a Pd-AntPhos catalyst that allows a metathesis-inactive allylic carbonate to serve as a masked terminal olefin, thereby enabling successive olefin metathesis events.
索拉芬 A 的全合成,一种粘细菌代谢产物和乙酰辅酶 A 羧化酶抑制剂,以 11 步(最长线性序列)完成,不到之前所需步骤的一半。 七种金属催化过程被用来实现步骤经济性(包括五个不对称过程和四个 C-C 键形成)。 目前的路线不使用手性助剂,并且五个 C-C 键形成中的四个利用非预金属化的伙伴。 为了最大限度地收敛,使用 Pd-AntPhos 催化剂开发了不对称 Tsuji 还原,该催化剂允许非聚合活性烯丙基碳酸酯作为掩蔽末端烯烃,从而能够进行连续的烯烃复分解反应。