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Polymer Chains Fold Prior to Crystallization.

Fan Jin1, Shichen Yuan1, Shijun Wang1

  • 1School of Polymer Science and Polymer Engineering, The University of Akron, Akron, Ohio 44325-3909, United States.

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|May 16, 2022
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Summary
This summary is machine-generated.

Polymer chain folding precedes crystallization, forming an adjacent re-entry structure. Subsequent melt and cold crystallization involve chain rearrangement within existing structures, not new folding.

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Area of Science:

  • Polymer Science
  • Materials Science
  • Physical Chemistry

Background:

  • The crystallization mechanism of polymers at the molecular level, specifically the sequence of chain folding versus lamellae formation, remains a subject of debate.
  • Understanding polymer chain behavior in both glassy and crystalline states is crucial for predicting material properties.

Purpose of the Study:

  • To investigate the local chain trajectory of polymers in rapidly quenched glassy states and thermodynamically stable crystals.
  • To determine whether chain folding or lamellae formation occurs first during polymer crystallization.
  • To elucidate the role of chain folding in melt and cold crystallization processes.

Main Methods:

  • Utilizing 13C-labeled semicrystalline polymers.
  • Employing 13C-13C double-quantum (DQ) nuclear magnetic resonance (NMR) spectroscopy to trace local chain trajectories.
  • Re-examining the natural abundance effect on DQ-NMR signals using extended chain conformations to accurately characterize glassy polymer chains.

Main Results:

  • Glassy polymer chains exhibit an adjacent re-entry structure (adjacent re-entry number, n = 1).
  • This adjacent re-entry structure is consistent with that observed in melt- and cold-grown crystals.
  • Local chain trajectory analysis revealed that folding precedes crystallization.

Conclusions:

  • Chain folding is an initial event that occurs before the formation of lamellar crystals.
  • Melt and cold crystallization processes primarily involve the rearrangement of pre-existing folded polymer chains rather than inducing further folding.