Visible Light-InducedC–H Alkylation of Azauracilswith <i>N</i>‑Hydroxyphthalimide Esters via CatalyticEDA Complex

Herein, we report sodium iodide (NaI)-catalyzed decarboxylative C–H alkylation of azauracils with <i>N</i>-hydroxyphthalimide (NHPI) esters facilitated by visible light activation of catalytic electron donor–acceptor (EDA) complexes. Control experiments and density functional theory calculations suggest that the decarboxylative coupling reaction proceeds via a transiently assembled EDA complex between the NHPI ester and NaI in <i>N</i>,<i>N</i>-dimethylacetamide solvent. This synthetic method efficiently applies to primary, secondary, and tertiary NHPI esters under mild, photocatalyst-free, and redox-neutral conditions, achieving high yields of the desired alkylated azauracils.