Incorporation of Dye‐Derived Carbon Dots Into Carbon Nitride Nanosheets for Enhanced Photoinduced 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.