Abstract
Electron donor-acceptor (EDA) complexes can
controllably generate radicals under mild conditions through selective
photoexcitation events. However, unproductive reactivity from fast deactivation
of the photoexcited complexes through back electron transfer has slowed the
development of EDA complexes in synthetic methodology. Here, we disclose the
study of EDA complexes derived from 2-methoxynaphthalene donor and acylated
ethyl isonicotinate N-oxide acceptor that undergo a fast N–O bond
fragmentation event upon photoexcitation. This reaction design not only
overcomes the limitations of back electron transfer but also enables the
regeneration of the donor species, representing a rare example EDA
photochemistry in a catalytic regime. The synthetic utility is demonstrated
through visible light-driven radical trifluoromethylation and Minisci
alkylation reactions. The scalability of the EDA complex promoted reaction evidenced
by the successful multigram-scale trifluoromethylation of methyl N-Boc
pyrrole-2-carboxylate in a continuous flow manifold.