Highly efficient dual photoredox/copper catalyzed atom transfer radical polymerization achieved through mechanism-driven photocatalyst design
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초록
내용
This study explores a novel photocatalyst (PC) for dual photoredox/copper ATRP that operates efficiently at sub-ppm levels. Utilizing PC design strategy, the research addresses high PC loadings' cost and purification challenges. By focusing on the ground state oxidation potential of PCs, which is crucial for PC regeneration, rather than their excited state reducing power for initiation, the study identifies optimal PC characteristics. Through screening PCs with different redox potentials and excited state properties, the team discovers 4DCDP-IPN, a PC with balanced excited state reducing power and high ground state oxidation potential. At just 50 ppb, this PC successfully synthesizes PMMA, achieving high conversion, narrow PDI, and excellent chain-end fidelity. The system demonstrates oxygen tolerance and feasibility for large-scale reactions under ambient conditions. This mechanism-driven PC design offers new insights into controlled radical polymerizations and broader metallaphotoredox applications.