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天然物Retrojusticidin B, Justicidin E和Helioxanthin之全合成研究
Dissertation

天然物Retrojusticidin B, Justicidin E和Helioxanthin之全合成研究

高子婷
Doctor of Philosophy (PHD), 國立清華大學, 化學系
2016

Abstract

自由基合環反應 合環反應 木酚素 呋喃 free radical cyclization annulation lignan furan
The dissertation is divided into two parts: Chapter I describes that a mild Pd/Cu-cocatalyzed radical cascade, proceeding via a sequence of Sonogashira coupling followed by [4 + 1] and [4 + 2] cycloadditions, has been developed to rapidly assemble cyclopenta[b]naphthalene and benzo[b]fluorene derivatives. In addition, a convenient and general approach for cyclopenta[b]naphthalene derivatives containing a structurally diverse functional group, including trimethyl silyl, aryl, ester, ketone, secondary/tertiary amide, phosphonate and halogen, at C-4 position has also been successfully developed, wherein Mn(III) plays a critical role to effect the oxidative tandem 5-exo-dig and 6-exo/endo cyclization efficiently. Finally, the total synthesis of natural products retrojusticidin B, justicidin E and helioxanthin, making use of a tandem free radical cyclization process mediated by Mn(OAc)3 as a key operation, has been concisely achieved in four or five steps in an overall yield of 45%, 33% and 44%. Charpter II describes that an efficient Cu(I)-catalyzed intramolecular cyclization of -activated carbonyl compounds has been developed, leading to 2,3,5-trisubstituted furans in good to high yields. The advantage of this synthetic method lies in its operational simplicity, mild reaction conditions and a wide scope of accessible substrates.

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