Structure‐Catalytic Activity in a Series of Push‐Pull Dicyanopyrazine/Dicyanoimidazole Photoredox Catalysts

A series of dicyanopyrazine and dicyanoimidazole derived push‐pull molecules have been prepared and further investigated as photoredox catalysts. The fundamental properties of the catalysts were studied by DSC, X‐ray analysis, absorption/emission spectra, and electrochemistry and were completed with the DFT results. The catalytic activity has been evaluated in visible light induced α‐functionalization of amines (cross‐dehydrogenative coupling and annulation reaction of tetrahydroisoquinolines). Thorough structure‐property‐catalytic activity relationships were elucidated. The developed series of tailored organic photoredox catalysts allows synthetic chemists to perform desired reactions under sustainable and mild conditions employing solely visible light as a source of energy.