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Types of Step-Growth Polymers: Polyesters01:20

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The introduction of polyesters has brought major development to the textile industry. The wrinkle-free behavior of polyester blends has eliminated the need for starching and ironing clothes.
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Solid-State Crosslinkable, Shape-Memory Polyesters Serving Tissue Engineering.

Jasper Delaey1, Laurens Parmentier1, Lincy Pyl2

  • 1Polymer Chemistry & Biomaterials group (PBM), Centre of Macromolecular Chemistry (CMaC), Department of Organic and Macromolecular Chemistry, Ghent University, Ghent, 9000, Belgium.

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New shape-memory polymers based on poly(D,L-lactide)/poly(ε-caprolactone) (PDLLA/PCL) copolymers exhibit tunable actuation temperatures and excellent shape recovery. These biocompatible polymers are suitable for additive manufacturing, showing great potential for biomedical applications.

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Area of Science:

  • Polymer Chemistry
  • Materials Science
  • Biomaterials Engineering

Background:

  • Developing advanced polymers with tunable properties is crucial for innovative applications.
  • Shape-memory polymers (SMPs) offer unique capabilities for smart devices and biomedical implants.
  • Poly(D,L-lactide)/poly(ε-caprolactone) (PDLLA/PCL) copolymers are promising biomaterials due to their biodegradability and tunable degradation rates.

Purpose of the Study:

  • To synthesize and characterize acrylate-endcapped PDLLA/PCL random copolymers with varying architectures and molar masses.
  • To investigate the influence of monomer content on the glass transition temperature and actuation behavior.
  • To evaluate the shape-memory properties, processability via additive manufacturing, and in vitro biocompatibility of the synthesized polymers.

Main Methods:

  • Synthesis of PDLLA/PCL random copolymers with acrylate end-caps in linear and star-shaped architectures.
  • Differential scanning calorimetry (DSC) to determine glass transition temperatures (Tg).
  • Mechanical testing to analyze viscoelastic behavior (storage modulus G').
  • Shape-memory testing to quantify shape recovery (Rr) and shape fixity (Rf).
  • Additive manufacturing techniques (DLP, 2PP, DPE) for polymer processing.
  • In vitro biocompatibility assays (MTS, live/dead staining) using human foreskin fibroblasts (HFFs).

Main Results:

  • PDLLA/PCL copolymers with tunable glass transition temperatures (10-42 °C) were synthesized by adjusting ε-caprolactone content (0-8 wt%).
  • Excellent shape-memory properties were achieved with high shape recovery (88-100%) and shape fixity (78-99.5%).
  • The polymers demonstrated successful processing via digital light processing, two-photon polymerization, and direct powder extrusion, retaining their shape-memory effect.
  • All synthesized polymers exhibited good in vitro biocompatibility, with high metabolic activity (≈100%) and cell viability (>70%) in direct contact with HFFs.

Conclusions:

  • Acrylate-endcapped PDLLA/PCL copolymers offer tunable thermal and mechanical properties for shape-memory applications.
  • These polymers can be effectively processed using various additive manufacturing techniques, enabling complex structure fabrication.
  • The demonstrated biocompatibility and excellent shape-memory performance make these materials highly promising for advanced biomedical devices and tissue engineering scaffolds.