Pd-catalyzed halocyclizations of unactivated 1,6-diynes through a formal anti-carbopalladation/bromi

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We report a Pd-catalyzed halocyclization of unactivated 1,6-diynes with N-bromosuccinimide (NBS).This approach produces stereo-defined dibromo substituted dihydropyrans,tetrahydropyridines,and 3-methylene cyclohexenes with exocyclic double bond appendages in mostly good yields.Copper salt was found to be a useful Lewis acid in this reaction.Mechanistically,a formal anti-carbopalladation and a bromide radical promoted PdⅡ-PdⅢ-PdⅠ-PdⅡ catalytic cycles were proposed to be involved in the formation of the dibromo-substituted products.Further functionalization of the dihydropyran derivatives underwent B(C6F5)3-catalyzed ring opening,and reduction afforded dibrominated 1,3-dienes with excellent stereoselectivity.
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