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A Truce–Smiles rearrangement of acyl‐anion equivalents generated by N‐heterocyclic carbene (NHC) catalysis has been achieved. The developed method includes CAr−O, CAr−S, or CAr−N bond cleavage for the formation of a CAr−C bond and enables access to 2‐hydroxybenzophenones, an important structural motif that is present in several bioactive natural products. By utilizing this procedure, the alkaloid...
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