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Intramolecular oxidative amination of readily accessible aminocyclooct‐4‐enes provides rapid and regioselective access to the 9‐azabicyclo[4.2.1]nonane framework characteristic of the natural product anatoxin‐a (1). This has enabled the synthesis of sp3‐rich chemical scaffolds suitable for diversification. A library of 881 lead‐like compounds is reported alongside a formal synthesis of anatoxin‐a...
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