Incorporation of Dye‐Derived Carbon Dots into Carbon Nitride Nanosheets for Enhanced Photoindcued Atom Transfer Radical Polymerization

Carbon dots have made significant advancements in photoinduced atom transfer radical polymerization (photo‐ATRP), achieving ultrafast reaction rates and precise control over the resulting polymers. However, their ultrasmall size necessitates time‐consuming and resource‐intensive purification steps, which can ultimately lead to undesirable product contamination. In this study, we integrated dye‐derived carbon dots (NCD) into nitrogen‐deficient carbon nitride (CN) nanosheets via a hydrothermal process, forming NCD@CN heterojunctions with an expanded delocalized heterocyclic structure, enhanced specific surface area and improved light absorption. The chemical linkages between the two components created NCD@CN heterojunctions, which improved interfacial interactions and promoted efficient charge transfer. The NCD@CN heterojunctions demonstrated ultrahigh activity, comparable to the NCD precursors, achieving a turnover number up to 1780 and a turnover frequency up to 59.3 min‐1. This led to the production of polymers with tailor‐made structures, predicted molecular weights and narrow dispersities. Additionally, they enabled complete catalyst recovery across multiple polymerization cycles. The incorporation of NCD into CN nanosheets affords new territory for high‐performance photocatalysts at the atomic level and provides alternative pathways for ultrafast photo‐ATRP processes.