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Total Synthesis of Euphane Triterpenoids Using Metal‐Catalyzed Hydrogen Atom Transfer
Author(s) -
Zhou Chengying,
Qin Weitian,
Tu Canhui,
Chen Yunxuan,
Fu Shaomin,
Liu Bo
Publication year - 2025
Publication title -
angewandte chemie
Language(s) - English
Resource type - Journals
eISSN - 1521-3757
pISSN - 0044-8249
DOI - 10.1002/ange.202503943
Subject(s) - catalysis , chemistry , metal , hydrogen , hydrogen atom , triterpenoid , combinatorial chemistry , stereochemistry , organic chemistry , alkyl
Abstract Euphane triterpenoids are widely distributed in nature and show various intriguing bioactivities, but relatively few synthetic routes to them have been described. Here, we report asymmetric convergent total syntheses of euphanes involving two triterpenoids and two nortriterpenoids: euphol, 25,26,27‐tris nor ‐3β‐hydroxy‐euphan‐24‐al, euphorbiumrin D, and 3‐oxo‐tirucall‐7‐ene‐3,20‐dione. The syntheses employ an enantioselective Antilla allylboration and intramolecular radical cyclization to construct ring A, a palladium‐catalyzed Liebeskind stannane‐thioester coupling to connect ring A with the bicyclic CD system, and a novel radical cascade with metal‐catalyzed hydrogen atom transfer (MHAT) to complete the polycyclic architecture. The late‐stage syntheses of both triterpenoids feature a diimide reduction and a MHAT/1,5‐hydrogen transfer cascade to diastereoselectively forge the C20 and C17 stereogenic centers.
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