Enantioselective Aza-Michael Addition of Imides by Using an Integrated Strategy Involving the Synthesis of a Family of Multifunctional Catalysts, Usage of Multiple Catalysis, and Rational Design of Experiment

A challenging asymmetric reaction (aza‐Michael addition of imides to enones) has been optimized through an integrated approach involving the synthesis of a family of organocatalysts, multiple catalysis (usage of additives), and finally with rational exploration of the chemical space by the application of the experiment design. Eureka! versus rational: No “eureka!” moment, but rather a rational step‐by‐step improvement. The optimization of a challenging reaction was achieved by using an integrated approach involving the synthesis of a family of organocatalysts, multiple catalysis, and through a rational exploration of chemical space with the application of the experiment design in asymmetric catalysis (see figure).