Understanding C−S bond photolysis of the thiocarbonylthio group for rapid synthesis of defect-free acrylic polymers without a photocatalyst
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Direct photolysis has emerged as a powerful synthetic tool for a wide range of applications, utilizing low-energy visible light without the need for costly photocatalysts or transition metals. A notable example is the photoiniferter, a controlled radical polymerization (CRP) that involves C−S photolysis as a crucial step. The photoiniferter exhibits unique characteristics not found in conventional CRP and finds applications in various fields. However, different reaction patterns are observed for different combinations of monomer−TCT−light irradiation conditions, and a comprehensive understanding of this phenomenon is lacking. In this study, we propose a mechanism for TCT photolysis through experimental and quantum chemical calculations. Based on these results, the reaction pattern was clearly understood according to monomer−TCT−light irradiation. By applying this theory, polyacrylates with minimal dead chains were also successfully synthesized in short reaction times.