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One-pot synthesis of hyperbranched polymers via visible light regulated switchable catalysis

Author

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  • Shuaishuai Zhu

    (Huazhong University of Science and Technology)

  • Maoji Zhao

    (Huazhong University of Science and Technology)

  • Hongru Zhou

    (Huazhong University of Science and Technology)

  • Yingfeng Wen

    (Huazhong University of Science and Technology)

  • Yong Wang

    (Huazhong University of Science and Technology)

  • Yonggui Liao

    (Huazhong University of Science and Technology)

  • Xingping Zhou

    (Huazhong University of Science and Technology)

  • Xiaolin Xie

    (Huazhong University of Science and Technology)

Abstract

Switchable catalysis promises exceptional efficiency in synthesizing polymers with ever-increasing structural complexity. However, current achievements in such attempts are limited to constructing linear block copolymers. Here we report a visible light regulated switchable catalytic system capable of synthesizing hyperbranched polymers in a one-pot/two-stage procedure with commercial glycidyl acrylate (GA) as a heterofunctional monomer. Using (salen)CoIIICl (1) as the catalyst, the ring-opening reaction under a carbon monoxide atmosphere occurs with high regioselectivity (>99% at the methylene position), providing an alkoxycarbonyl cobalt acrylate intermediate (2a) during the first stage. Upon exposure to light, the reaction enters the second stage, wherein 2a serves as a polymerizable initiator for organometallic-mediated radical self-condensing vinyl polymerization (OMR-SCVP). Given the organocobalt chain-end functionality of the resulting hyperbranched poly(glycidyl acrylate) (hb-PGA), a further chain extension process gives access to a core-shell copolymer with brush-on-hyperbranched arm architecture. Notably, the post-modification with 2,2,6,6-tetramethylpiperidine-1-oxyl (TEMPO) affords a metal-free hb-PGA that simultaneously improves the toughness and glass transition temperature of epoxy thermosets, while maintaining their storage modulus.

Suggested Citation

  • Shuaishuai Zhu & Maoji Zhao & Hongru Zhou & Yingfeng Wen & Yong Wang & Yonggui Liao & Xingping Zhou & Xiaolin Xie, 2023. "One-pot synthesis of hyperbranched polymers via visible light regulated switchable catalysis," Nature Communications, Nature, vol. 14(1), pages 1-9, December.
  • Handle: RePEc:nat:natcom:v:14:y:2023:i:1:d:10.1038_s41467-023-37334-x
    DOI: 10.1038/s41467-023-37334-x
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    References listed on IDEAS

    as
    1. Jiaxi Xu & Xin Wang & Nikos Hadjichristidis, 2021. "Diblock dialternating terpolymers by one-step/one-pot highly selective organocatalytic multimonomer polymerization," Nature Communications, Nature, vol. 12(1), pages 1-10, December.
    2. Robert M. Jacobberger & Vikram Thapar & Guang-Peng Wu & Tzu-Hsuan Chang & Vivek Saraswat & Austin J. Way & Katherine R. Jinkins & Zhenqiang Ma & Paul F. Nealey & Su-Mi Hur & Shisheng Xiong & Michael S, 2020. "Boundary-directed epitaxy of block copolymers," Nature Communications, Nature, vol. 11(1), pages 1-10, December.
    3. Tim Stößer & Gregory S. Sulley & Georgina L. Gregory & Charlotte K. Williams, 2019. "Easy access to oxygenated block polymers via switchable catalysis," Nature Communications, Nature, vol. 10(1), pages 1-9, December.
    4. Yuwei Gu & Eric A. Alt & Heng Wang & Xiaopeng Li & Adam P. Willard & Jeremiah A. Johnson, 2018. "Photoswitching topology in polymer networks with metal–organic cages as crosslinks," Nature, Nature, vol. 560(7716), pages 65-69, August.
    5. Yangtian Lu & Takashi Nemoto & Masatoshi Tosaka & Shigeru Yamago, 2017. "Synthesis of structurally controlled hyperbranched polymers using a monomer having hierarchical reactivity," Nature Communications, Nature, vol. 8(1), pages 1-8, December.
    6. Yuwei Gu & Eric A. Alt & Heng Wang & Xiaopeng Li & Adam P. Willard & Jeremiah A. Johnson, 2018. "Publisher Correction: Photoswitching topology in polymer networks with metal–organic cages as crosslinks," Nature, Nature, vol. 563(7729), pages 17-17, November.
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