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Controlling Enzymatic Polymerization from Surfaces with Switchable Bioaffinity.

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Surface protein affinity controls polymer brush synthesis via surface-initiated biocatalytic atom transfer radical polymerization (SI-bioATRP). This method allows precise control over polymer film functionalization by tuning protein-surface interactions.

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Area of Science:

  • Polymer Chemistry
  • Biocatalysis
  • Surface Science

Background:

  • Protein-surface affinity is crucial for controlling polymer brush synthesis.
  • Surface-initiated biocatalytic atom transfer radical polymerization (SI-bioATRP) offers a pathway for polymer grafting.
  • Hemoglobin (Hb) acts as an "ATRPase" catalyst in these polymerizations.

Purpose of the Study:

  • To investigate how protein-surface affinity governs SI-bioATRP.
  • To demonstrate controlled synthesis of polymer brushes by modulating protein-polymer interactions.
  • To explore the use of thermoresponsive polymers and pH-dependent enzyme activity for controlled polymerization.

Main Methods:

  • Utilizing surface-initiated biocatalytic atom transfer radical polymerization (SI-bioATRP).
  • Employing thermoresponsive poly(N-isopropylacrylamide) (PNIPAM) brushes.
  • Regulating polymerization by temperature changes relative to the lower critical solution temperature (LCST).
  • Modulating hemoglobin (Hb) activity via pH-induced conformational changes.

Main Results:

  • Polymer brush thickness was controlled in discrete steps by switching temperature above and below LCST.
  • Multistep SI-bioATRP achieved high control, chain end fidelity, and enabled multiblock copolymer synthesis in aqueous conditions.
  • Acidic pH accelerated Hb activity by inducing a transition to a molten globule conformation, enhancing polymerization.
  • Demonstrated precise control over grafted polymer film synthesis by modulating protein-surface affinity.

Conclusions:

  • Multistep SI-bioATRP provides a controlled method for synthesizing polymer brushes and films.
  • Modulating interfacial physicochemical properties, specifically protein-surface affinity, is key to controlling biocatalytic polymerization.
  • This approach offers a novel strategy for material functionalization by leveraging bioadhesion principles.