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This work first discloses a new strategy for amine activation to give reactive amine anion by in situ generated iminium cation‐amine anion pair through decomposition of sterically hindered aminals. Utilizing this strategy, a highly regio‐ and chemoselective cyclocarboamination of ortho‐formyl phenylacetylenes with secondary amines has been realized under metal‐free mild reaction conditions. The cyclocarboamination...
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