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Regio- and Stereoselective Biocatalytic Monoamination of a Triketone Enables Asymmetric Synthesis of Both Enantiomers of the Pyrrolizidine Alkaloid Xenovenine Employing Transaminases

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논문

Regio- and Stereoselective Biocatalytic Monoamination of a Triketone Enables Asymmetric Synthesis of Both Enantiomers of the Pyrrolizidine Alkaloid Xenovenine Employing Transaminases

학술지

Advanced synthesis & catalysis

저자명

Payer, Stefan E.; Schrittwieser, Joerg H.; Grischek, Barbara; Simon, Robert C.; Kroutil, Wolfgang

초록

<P><B>Abstract</B></P><P>The (+)&#8208; as well as the (&minus;)&#8208;enantiomer of the pyrrolizidine alkaloid xenovenine were prepared within five steps with 17 and 30% overall yields, respectively, in optically pure form, >99% <I>ee</I> as well as >99% <I>de</I>. In the asymmetric key step a transaminase performed a regio&#8208; and stereoselective monoamination of a triketone. By employing two enantiocomplementary transaminases from <I>Arthrobacter</I> sp. both enantiomers were accessible. The triketone was readily prepared <I>via</I> two steps starting from commercially available, achiral 2&#8208;(<I>n</I>&#8208;heptyl)furan. In the final catalytic hydrogenation step, the newly introduced chiral centre directed hydrogen addition to form preferentially the desired (5<I>Z</I>,8<I>E</I>)&#8208;diastereomer. The regio&#8208; and stereoselective amination of a single ketone moiety out of three allowed the performance of the shortest and highest yielding total synthesis of the bicyclic showcase pyrrolizidine alkaloid without the need for protecting strategies.</P>

발행연도

2016

발행기관

WILEY&#x2010;VCH Verlag

ISSN

1615-4150

ISSN

1615-4169

358

3

페이지

pp.444-451

주제어

amination; biocatalysis; biotransformations; pyrrolizidine alkaloids; transaminases; xenovenine

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1 2023-12-11
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논문; 2015-12-09

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