Uniform macromolecular networks by end-to-end click chemistry between discrete tetrahedral star macromolecules
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초록
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Cross-linking via click chemistry of multi-arm star polymers creates polymer networks with minimal inhomogeneities. Here, we report the synthesis of discrete tetrahedral star macromolecules (dTSMs) composed of polylactide (PLA) arms with discrete molecular weight. A set of dTSMs equipped with end groups for Cu-free strain-promoted cyclooctyne-azide click chemistry (SPAAC) was prepared. End-to-end click reaction resulted in the formation of networks with a high degree of swelling without sacrificing mechanical robustness. The structural details were investigated by network disassembly spectrometry (NDS). By implementing a cleavable repeating unit in the PLA arms in a sequence-specific manner, the networks could be disassembled into fragments having discrete molecular weights representing the connectivity in the network. This NDS analysis confirmed that end-to-end click reactions of dTSMs resulted in the formation of an ideal network above the critical concentration of building blocks.