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Fibers 2015, 3(3), 348-372; doi:10.3390/fib3030348

Influence of pH on Morphology and Structure during Hydrolytic Degradation of the Segmented GL-b-[GL-co-TMC-co-CL]-b-GL Copolymer

1
Chemical Engineering Department, Polytechnic University of Catalonia, Av. Diagonal 647, Barcelona E-08028, Spain
2
Braun Surgical S.A., Carretera de Terrassa 121, Barcelona 08191, Spain
3
ALBA Synchrotron Light Facility, Ctra BP 1413 km 3.3, Cerdanyola del Vallès, Barcelona 08290, Spain
*
Author to whom correspondence should be addressed.
Academic Editor: Jingwei Xie
Received: 24 July 2015 / Accepted: 8 September 2015 / Published: 15 September 2015
(This article belongs to the Special Issue Fibers for Biomedical Applications)
View Full-Text   |   Download PDF [1660 KB, uploaded 15 September 2015]   |  

Abstract

Hydrolytic degradation in media having a continuous variation of pH from 2 to 12 was studied for a copolymer having two polyglycolide hard blocks and a middle soft segment constituted by glycolide, trimethylene carbonate, and ɛ-caprolactone units. The last units were susceptible to cross-linking reactions by γ irradiation that led to an increase of the molecular weight of the sample. Nevertheless, the susceptibility to hydrolytic degradation was enhanced with respect to non-irradiated samples and consequently such samples were selected to analyze the degradation process through weight loss measurements and the evaluation of changes on molecular weight, morphology, and SAXS patterns. Results reflected the different hydrolytic mechanisms that took place in acid and basic media and the different solubilization of the degradation products. Thus, degradation was faster and solubilization higher in the basic media. In this case, fibers showed a high surface erosion and the formation of both longitudinal and deep circumferential cracks that contrasted with the peeling process detected at intermediate pHs (from 6 to 8) and the absence of longitudinal cracks at low pHs. SAXS measurements indicated that degradation was initiated through the hydrolysis of the irregular molecular folds placed on the amorphous interlamellar domains but also affected lamellar crystals at the last stages. Subsequent heating processes performed with degraded samples were fundamental to reveal the changes in microstructure that occurred during degradation and even the initial lamellar arrangement. In particular, the presence of interfibrillar domains and the disposition of lamellar domains at different levels along the fiber axis for a determined cross-section were evidenced. View Full-Text
Keywords: absorbable sutures; glycolide copolymer; hydrolytic degradation; γ-irradiation; lamellar microstructure; small angle X-ray scattering absorbable sutures; glycolide copolymer; hydrolytic degradation; γ-irradiation; lamellar microstructure; small angle X-ray scattering
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This is an open access article distributed under the Creative Commons Attribution License which permits unrestricted use, distribution, and reproduction in any medium, provided the original work is properly cited. (CC BY 4.0).

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MDPI and ACS Style

Márquez, Y.; Martínez, J.C.; Turon, P.; Franco, L.; Puiggalí, J. Influence of pH on Morphology and Structure during Hydrolytic Degradation of the Segmented GL-b-[GL-co-TMC-co-CL]-b-GL Copolymer. Fibers 2015, 3, 348-372.

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