Polarity‐Directed One‐Pot Asymmetric Cascade Reactions Mediated by Two Catalysts in an Aqueous Buffer

A crossing between phases: Polarity makes a difference in distinguishing substrates of otherwise nearly identical chemical reactivities. A one-pot cascade reaction involving nitromethane and two aliphatic aldehydes with similar reactivities has been developed (see scheme). The use of a biphasic reaction medium with two different organic catalysts results in the controlled incorporation of both aldehyde substrates into a single major cross-product.