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The aromatic nitrogen atoms of heteroarylaldehydes are activated by carbene catalysts to react with ketone electrophiles. Multi‐functionalized cyclic N,O‐acetal products are afforded in good to excellent yields and optical purities. Our reaction involves the formation of an unprecedented aza‐fulvene‐type acylazolium intermediate. A broad range of N‐heteroaromatic aldehydes and electron‐deficient ketone...
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