Abstract

We have investigated the structural response of melt-spun poly-3-hydroxybutyrate (P3HB) fibers to stress and temperature and its impact on the mechanical properties. Low-stress (≤1.6 MPa, 100–130 °C) annealed P3HB fibers showed a considerable viscoelastic behavior and remained ductile up to at least two months. Stress annealing with high weights (≥32 MPa), however, lead to fibers with a higher tensile strength (182 MPa) and with a lower elongation at break (22%). These significant differences in the tensile properties are closely related to structural changes, which we have studied with in-situ wide-angle x-ray diffraction (WAXD) and small-angle x-ray scattering (SAXS) experiments. A highly oriented non-crystalline mesophase (Pnc), which is located in-between orthorhombic α-crystals is growing during high-stress annealing but disappears during low-stress annealing. However, it is possible to restore the mesophase by post-drawing. The viscoelastic hysteresis behavior of low-stress annealed fibers is explained by a reversible transformation of α-crystals into mesophase and back.

Highlights

  • Poly-3-hydroxybutyrate (P3HB) is a thermoplastic poly­ hydroxyalkanoate (PHA), which is biodegradable and of spe­ cific interest for biomedical applications such as tissue engineering scaffolds, bone and cartilage scaffolds, drug delivery, sutures or wound dressing [1,2,3,4,5,6]

  • These significant differences in the tensile properties are closely related to structural changes, which we have studied with in-situ wide-angle x-ray diffraction (WAXD) and small-angle xray scattering (SAXS) experiments

  • In order to better understand the impact of annealing procedures on the structure and its interplay with the mechanical properties, we have explored the structural response of melt-spun P3HB fibers to low-stress annealing ( 16 MPa) and to high-stress annealing ( 32 MPa) with insitu wide-angle x-ray diffraction (WAXD) and small-angle x-ray scat­ tering (SAXS) experiments

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Summary

Introduction

Poly-3-hydroxybutyrate (P3HB) is a thermoplastic poly­ hydroxyalkanoate (PHA), which is biodegradable and of spe­ cific interest for biomedical applications such as tissue engineering scaffolds, bone and cartilage scaffolds, drug delivery, sutures or wound dressing [1,2,3,4,5,6] For such future applications, it is crucial to tailor the mechanical properties of P3HB fibers in order to fulfill specific re­ quirements regarding tenacity and elasticity. We have obtained stable P3HB monofilaments by an up-scalable meltspinning method, where the take-up godet was installed at an unusually short distance from the spinneret [7] These monofilaments consist of a network of longitudinally oriented lamellae (α-crystals) that are embedded in the amorphous phase. The orthorhombic α-crystals are formed by molecular chains that adopt the 21 helix conformation [8]

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