3 years ago

Enzymatic Cascade Catalysis for the Synthesis of Multiblock and Ultrahigh-Molecular-Weight Polymers with Oxygen Tolerance

Enzymatic Cascade Catalysis for the Synthesis of Multiblock and Ultrahigh-Molecular-Weight Polymers with Oxygen Tolerance
Zesheng An, Yue Lv, Zhifen Liu
Synthesis of well-defined multiblock and ultrahigh-molecular-weight (UHMW) polymers has been a perceived challenge for reversible-deactivation radical polymerization (RDRP). An even more formidable task is to synthesize these extreme polymers in the presence of oxygen. A novel methodology involving enzymatic cascade catalysis is developed for the unprecedented synthesis of multiblock polymers in open vessels with direct exposure to air and UHMW polymers in closed vessels without prior degassing. The success of this methodology relies on the extraordinary deoxygenation capability of pyranose oxidase (P2Ox) and the mild yet efficient radical generation by horseradish peroxidase (HRP). The facile and green synthesis of multiblock and UHMW polymers using biorenewable enzymes under environmentally benign and scalable conditions provides a new pathway for developing advanced polymer materials. Ultrahigh: Enzymatic cascade catalysis enables the synthesis of multiblock (up to 10 blocks) copolymers and ultrahigh-molecular-weight polymers (UHMW; up to 2.3×106 g mol−1). The reaction employs a P2Ox-HRP system and can be run in vessels open to air, thus highlighting the oxygen tolerance of the process. P2Ox=pyranose oxidase, HRP=horseradish peroxidase, ACAC=acetylacetone, RAFT=reversible addition-fragmentation chain transfer.

Publisher URL: http://onlinelibrary.wiley.com/resolve/doi

DOI: 10.1002/anie.201707993

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