Journal
POLYMER CHEMISTRY
Volume 10, Issue 19, Pages 2477-2483Publisher
ROYAL SOC CHEMISTRY
DOI: 10.1039/c9py00213h
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Funding
- NSF DMR [1436219, 1436201]
- DoE [ER 45998]
- NSF [CHE-9808188, CHE-1039870, CHE-1726525]
- Direct For Mathematical & Physical Scien
- Division Of Materials Research [1436219, 1436201] Funding Source: National Science Foundation
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This work explores the concept of structurally tailored and engineered macromolecular (STEM) networks by proposing a novel metal-free approach to prepare the networks. STEM networks are composed of polymer networks with latent initiator sites affording post-synthesis modification. The proposed approach relies on selectively activating the fragmentation of trithiocarbonate RAFT agent by relying on visible light RAFT iniferter photolysis coupled with RAFT addition-fragmentation process. The two-step synthesis explored in this work generates networks that are compositionally and mechanically differentiated than their pristine network. In addition, by careful selection of crosslinkers, conventional poly(ethylene glycol) dimethacrylate (Mn = 750) or trithiocarbonate dimethacrylate crosslinker (bis[(2-propionate) ethyl methacrylate] trithiocarbonate (bisPEMAT)), and varying concentrations of RAFT inimer (2-(2-(n-butyltrithiocarbonate)- propionate) ethyl methacrylate (BTPEMA)), three different types of primary (STEM-0) poly(methyl methacrylate) (PMMA) networks were generated under green light irradiation. These networks were then modified with methyl acrylate (MA) or N, N-dimethylacrylamide (DMA), under blue light irradiation to yield STEM-1 gels that are either stiffer or softer with different responses to polarity (hydrophilicity/hydrophobicity).
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