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A general and enantioselective N‐heterocyclic carbene (NHC)‐catalyzed lactonization of simple enals and α‐ketoesters has been discovered using a new ternary cooperative catalytic system. The highly selective annulation was achieved by using a combination of a chiral NHC, a hydrogen‐bond donor, and a metal salt, facilitating self‐assembly of the reactive partners. A proposed model for this new mode...
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