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An Alkyne‐Metathesis‐Based Approach to the Synthesis of the Anti‐Malarial Macrodiolide Samroiyotmycin A

Ektoras Yiannakas, Mark I. Grimes, James T. Whitelegge, Alois Fürstner, Alison N. Hulme

2021Angewandte Chemie International Edition42 citationsDOIOpen Access PDF

Abstract

Abstract We report the first total synthesis of samroiyotmycin A ( 1 ), a C 2 ‐symmetric 20‐membered anti‐malarial macrodiolide isolated from Streptomyces sp. The convergent synthetic strategy orchestrates bisalkyne fragment‐assembly using an unprecedented Schöllkopf‐type condensation on a substituted β‐lactone and an ambitious late‐stage one‐pot alkyne cross metathesis–ring‐closing metathesis (ACM–RCAM) reaction. The demanding alkyne metathesis sequence is achieved using the latest generation of molybdenum alkylidynes endowed with a tripodal silanolate ligand framework. Subsequent conversion to the required E‐alkenes uses contemporary hydrometallation chemistry catalysed by tetrameric cluster [{Cp*RuCl} 4 ].

Topics & Concepts

AlkyneMetathesisConvergent synthesisRing-closing metathesisCombinatorial chemistryStereochemistryChemistrySalt metathesis reactionSequence (biology)Ligand (biochemistry)Total synthesisOrganic chemistryCatalysisReceptorPolymerPolymerizationBiochemistrySynthetic Organic Chemistry MethodsMicrobial Natural Products and BiosynthesisChemical Synthesis and Analysis
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