Journal
MACROMOLECULES
Volume 52, Issue 15, Pages 5538-5545Publisher
AMER CHEMICAL SOC
DOI: 10.1021/acs.macromol.9b00940
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Funding
- TJ Park Science Fellowship of POSCO TJ Park Foundation
- Basic Science Research Program through the National Research Foundation of Korea (NRF) - Ministry of Education [NRF-2016R1D1A1B03936002]
- Fundamental Research Program of KIMS [PNK6320]
- Spanish Ministry for Science (MINECO-FEDER) [CTQ2017-87054, RTI2018-097508-B-100]
- Severo Ochoa program for Centers of Excellence in RD (MINECO) [SEV-2016-0686]
- Comunidad de Madrid [2018/NMT4511]
- Campus of International Excellence (CET) UAM+CSIC
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A highly efficient organic photocatalyst (OPC) for photoinduced electron/energy-transfer reversible addition-fragmentation chain-transfer (PET-RAFT) polymerization was identified through a systematic catalyst design and discovery. The devised OPC offers excellent control over PET-RAFT polymerizations of methyl methacrylate at very low catalyst loadings (5 ppm), that is, ca. 5-50 times lower loadings than other OPCs reported so far. Moreover, excellent oxygen tolerance was achieved using the discovered OPC combined with trithiocarbonate-based chain-transfer agent (CTA) under low-energy light irradiation conditions. In depth experimental and computational investigations revealed that (1) strong visible-light absorption and efficient generation of long-lived triplet states of the OPC due to its unique molecular structure and (2) the oxidation stability and no rate retardation of trithiocarbonate-based CTA are the key to the outstanding oxygen tolerance and ppm-level catalyst loadings. Our approach is thus believed to address a variety of challenging tasks related to polymer synthesis and living additive manufacturing.
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