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Sequence-controlled polymers can now be precisely synthesized and selectively depolymerized using enzymes. This breakthrough enables circular recycling of advanced polymer materials by preserving encoded molecular information.

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Area of Science:

  • Polymer Chemistry
  • Biocatalysis
  • Materials Science

Background:

  • Sequence-controlled polymers offer precise structural and functional control but face synthesis and end-of-life challenges.
  • Current depolymerization methods lack regioselectivity, leading to information loss and limiting polymer circularity.
  • Enzymatic catalysis presents a promising avenue for selective polymer bond cleavage due to substrate specificity.

Purpose of the Study:

  • To synthesize and characterize a sequence-controlled copolyamide, poly(X,AMA), with precise repeat-unit ordering.
  • To investigate the regioselective enzymatic depolymerization of poly(X,AMA) using Nylon hydrolase homologues.
  • To establish enzymatic depolymerization as a viable strategy for the circular recycling of sequence-controlled polymers.

Main Methods:

  • Synthesis of poly(X,AMA) via solid-state polycondensation (SSP) of sequence-defined oligomers.
  • Characterization of polymer microstructure and sequence fidelity using 13C NMR and MALDI-TOF mass spectrometry.
  • Screening of 96 Nylon hydrolase homologues for regioselective depolymerization and computational modeling of enzyme-substrate interactions.

Main Results:

  • Poly(X,AMA) exhibited distinct crystallinity, morphology, and thermal behavior compared to statistical copolymers and Nylon-66, attributed to sequence control.
  • Enzymatic screening revealed significant sequence selectivity, with specific enzymes preferentially releasing defined tetrads (XAMA or MAXA).
  • Computational modeling elucidated structural features responsible for the observed regioselectivity in enzymatic depolymerization.

Conclusions:

  • Selective enzymatic depolymerization is a viable strategy for the circular recycling of sequence-controlled polymers.
  • The study provides a foundation for engineering enzymes for programmable polymer deconstruction and advancing polymer circularity.
  • Precise control over polymer sequence translates to controllable degradation pathways.