Litcius/Paper detail

Total Synthesis of the Hexacyclic Sesterterpenoid Niduterpenoid B via Structural Reorganization Strategy

Yuan Xue, Si‐Hua Hou, Xiang Zhang, Fu‐Min Zhang, Xiao‐Ming Zhang, Yong‐Qiang Tu

2024Journal of the American Chemical Society29 citationsDOI

Abstract

To date, it remains challenging to precisely and efficiently construct structurally intriguing polycarbocycles with densely packed stereocenters in organic synthesis. Niduterpenoid B, a naturally occurring ERα inhibitor, exemplifies this complexity with its intricate polycyclic network comprising 5 cyclopentane and 1 cyclopropane rings, featuring 13 contiguous stereocenters, including 4 all-carbon quaternary centers. In this work, we describe the first total synthesis of niduterpenoid B using a structural reorganization strategy. Key features include the following: (1) an efficient methoxy-controlled cascade reaction that precisely forges a highly functionalized tetraquinane (A-D rings) bearing sterically hindered contiguous quaternary stereocenters; (2) a rhodium-catalyzed [1 + 2] cycloaddition that facilitates the construction of a strained 3/5 bicycle (E-F rings) angularly fused with ring D.

Topics & Concepts

StereocenterChemistryCyclopentaneRing (chemistry)StereochemistryCycloadditionTotal synthesisSteric effectsCyclopropaneRhodiumCatalysisEnantioselective synthesisOrganic chemistryCyclopropane Reaction MechanismsSynthetic Organic Chemistry MethodsPlant biochemistry and biosynthesis