Ricardo I. Rodríguez, Julien Paut, Giona Armellin, Stefano Visentini, Gabriel Cormier, Federico Droghetti, Mirco Natali, Marco Bortolus, Giorgio Pelosi, Luca Dell’ Amico
The activation of amines into thiocarbamoyl fluorides (TCarbFs) provides access to valuable nitrogen-based functionalities. However, their broader use has been hindered by the reliance on harsh reagents and conditions. Here we report a photochemical method for in situ generation of thiocarbonyl difluoride (TCF) from N-trifluoromethylthiophthalimide (Phth–SCF₃) using visible light and organic reductants. This strategy allows the synthesis of structurally complex azetidines from strained azabicyclo[1.1.0]butanes (ABBs). TCF-mediated ring opening followed by semipinacol rearrangement or nucleophilic additions enables direct access to spiro- and fluorinated TCarbF-azetidines in a single step. Mechanistic studies support a single-electron reduction pathway and rationalize the impact of the photocatalyst on the observed selectivity. The discovery offers a general platform for amine activation and addresses a long-standing gap in azetidine functionalization. The activation of amines into thiocarbamoyl fluorides provides access to valuable nitrogen-based functionalities. Here, the authors report a mild, photochemical method for in-situ generation of thiocarbonyl difluoride from N-trifluoromethylthiophthalimide using visible light and organic reductants, and apply this strategy to the synthesis of azetidines from strained azabicyclo[1.1.0]butanes.