A Multifunctional Photoredox-Organocatalyst System for Small Molecule Activation

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Homogeneous photoredox catalysis offers an intriguing alternative to traditional thermally-promoted reactions.1 These photochemically driven processes use an abundant, cheap energy source (the sun or ambient light) under mild reactions conditions and employ well-defined catalysts that act to efficiently harness photochemical energy. Typical photoredox catalysts (PRC) consist of RuII or IrIII complexes, though other photophysically active complexes based on AuI, ReI, CuI and PtII have all been explored. Few studies have systematically probed the optoelectronic properties of the catalysts or designed bespoke PRCs in order to tune their reactivity.This proposal targets the synthesis, design and application of organic TADF compounds as PRCs with the following goals: 1) design and synthesis of very high triplet energy PRCs; 2) utilization of these PRCs for reduction of aryl chlorides and alkyl halides that is currently generally not applicable; 3) further increase reactivity through dual substrate activation with an organocatalyst; 4) design an all-in-one system that contains both the PRC and organocatalyst functionality.