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The conversion of alkenes to macromolecules called polymers is a reaction of high commercial importance. The structure of the polymer is defined by a repeating unit, while the terminal groups are considered insignificant. The average degree of polymerization represents the number of repeating units in the polymer molecule and is denoted by the subscript n.
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The polymerization process that involves carbanion as an intermediate is called anionic polymerization. It is also a type of addition or chain-growth polymerization. Anionic polymerization gets initiated by a strong nucleophile such as an organolithium or a Grignard reagent. The most commonly used initiator for anionic polymerization is butyl lithium. Monomers involved in anionic polymerization must possess a vinyl group bonded to one or two electron-withdrawing groups. For instance,...
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Polymers are classified as linear or branched on the basis of their chain architecture. The polymer chains in linear polymers have a long chain-like structure with minimal to no branching at all. Even if a polymer features large substituent groups on the monomer, which appear as branches to the skeleton, it is not considered a branched polymer. A branched polymer contains secondary polymer chains that arise from the main polymer chain. The branching occurs when the polymer growth shifts from...
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The Preparation and Properties of Thermo-reversibly Cross-linked Rubber Via Diels-Alder Chemistry
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Dynamic Aliphatic Polyester Elastomers Crosslinked with Aliphatic Dianhydrides.

Marianne S Meyersohn1, Farihah M Haque1, Marc A Hillmyer1

  • 1Department of Chemistry, University of Minnesota, Minneapolis, Minnesota 55455, United States.

ACS Polymers Au
|October 16, 2023
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Summary
This summary is machine-generated.

This study developed reprocessable, high-performance elastomers from bio-based poly(γ-methyl-ε-caprolactone) using dynamic covalent chemistry. These novel materials offer tunable properties for advanced engineering applications.

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Area of Science:

  • Polymer Chemistry
  • Materials Science
  • Sustainable Materials

Background:

  • Chemically crosslinked elastomers are vital in adhesives and sealants but typically lack reprocessability.
  • Poly(γ-methyl-ε-caprolactone) (PγMCL) is a bio-sourced, degradable polyester with potential for elastomer applications.
  • Dynamic covalent bonds offer a pathway to create reprocessable crosslinked materials.

Purpose of the Study:

  • To investigate the dynamic behavior and mechanical properties of PγMCL elastomers crosslinked with aliphatic dianhydrides.
  • To explore the potential for reprocessing these novel elastomer materials.
  • To establish structure-property relationships for high-performance elastomer design.

Main Methods:

  • Synthesis of PγMCL elastomers using specific dianhydride crosslinkers and star polymers.
  • Stress relaxation experiments to determine viscosity and activation energy.
  • Dynamic mechanical thermal analysis and rheological studies to probe network dynamics.
  • Tensile testing to evaluate mechanical properties like Young's modulus and strain at break.

Main Results:

  • Elastomers exhibited Arrhenius-dependent viscosity with an activation energy of 118 ± 8 kJ/mol, consistent with transesterification.
  • Dynamic mechanical and rheological analyses confirmed the dynamic nature of the crosslinked networks.
  • Tensile tests revealed materials with high strain at break and low Young's moduli, characteristic of soft, strong elastomers.
  • The developed elastomers demonstrated potential for reprocessing at moderately elevated temperatures.

Conclusions:

  • PγMCL elastomers crosslinked with aliphatic dianhydrides exhibit dynamic covalent behavior.
  • The materials possess desirable mechanical properties for soft and strong elastomer applications.
  • Controlling exchange chemistry and macromolecular structure enables the creation of high-performance, reprocessable elastomers.