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Selection Rules: Photochemical Activation
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We developed a supramolecular near-infrared photoenzyme (SNIRPE) system for efficient polymer synthesis. This system overcomes limitations in traditional methods, enabling the creation of ultrahigh molecular weight polymers with high precision.

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Area of Science:

  • Polymer Chemistry
  • Biomaterials Science
  • Photocatalysis

Background:

  • Near-infrared (NIR) irradiation offers advantages for photocontrolled radical polymerization, including spatiotemporal precision, deep tissue penetration, and biocompatibility.
  • Current NIR polymerization methods suffer from low efficiency and limited access to high-molecular-weight polymers, hindering their practical application.

Purpose of the Study:

  • To develop a novel system for efficient and controlled NIR-driven radical polymerization.
  • To overcome the limitations of low efficiency and restricted molecular weight achievable with existing NIR polymerization techniques.

Main Methods:

  • A supramolecular NIR photoenzyme (SNIRPE) system was designed, integrating glucose oxidase (GOx) for enzymatic deoxygenation and tetrasulfonated zinc phthalocyanine (ZnPcS4-) for photoredox catalysis.
  • A spatially confined cascade mechanism was employed: GOx generates H2O2, which is then photodecomposed by ZnPcS4- under NIR irradiation to produce hydroxyl radicals (•OH).
  • This approach facilitated oxygen-tolerant, high-throughput reversible addition-fragmentation chain transfer (RAFT) polymerization across various volumes (µL to 100 mL).

Main Results:

  • The SNIRPE system achieved ultrahigh molecular weights (UHMWs, Mn > 1000 kg mol−1, Đ < 1.20) with exceptionally low catalyst loadings (50 ppb ZnPcS4−), significantly outperforming conventional NIR photoredox systems.
  • Scalability was demonstrated via 100 mL batch synthesis, and polymerization through porcine tissue highlighted the system's biomedical potential.
  • The method proved effective for oxygen-tolerant RAFT polymerization, enabling high-throughput synthesis.

Conclusions:

  • The developed SNIRPE system effectively combines enzymatic efficiency with photoredox versatility to address longstanding challenges in NIR-driven polymer synthesis.
  • This approach enables the production of ultrahigh molecular weight polymers with unprecedented efficiency and control under NIR irradiation.
  • The system's scalability and demonstrated utility in biological tissues pave the way for advanced applications in polymer science and biomedicine.