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Tuning the degradation profiles of poly(L-lactide)-based materials through miscibility.

ABSTRACT: The effective use of biodegradable polymers relies on the ability to control the onset of and time needed for degradation. Preferably, the material properties should be retained throughout the intended time frame, and the material should degrade in a rapid and controlled manner afterward. The degradation profiles of polyester materials were controlled through their miscibility. Systems composed of PLLA blended with poly[(R,S)-3-hydroxybutyrate] (a-PHB) and polypropylene adipate (PPA) with various molar masses were prepared through extrusion. Three different systems were used: miscible (PLLA/a-PHB5 and PLLA/a-PHB20), partially miscible (PLLA/PPA5/comp and PLLA/PPA20/comp), and immiscible (PLLA/PPA5 and PLLA/PPA20) blends. These blends and their respective homopolymers were hydrolytically degraded in water at 37 °C for up to 1 year. The blends exhibited entirely different degradation profiles but showed no diversity between the total degradation times of the materials. PLLA presented a two-stage degradation profile with a rapid decrease in molar mass during the early stages of degradation, similar to the profile of PLLA/a-PHB5. PLLA/a-PHB20 presented a single, constant linear degradation profile. PLLA/PPA5 and PLLA/PPA20 showed completely opposing degradation profiles relative to PLLA, exhibiting a slow initial phase and a rapid decrease after a prolonged degradation time. PLLA/PPA5/comp and PLLA/PPA20/comp had degradation profiles between those of the miscible and the immiscible blends. The molar masses of the materials were approximately the same after 1 year of degradation despite their different profiles. The blend composition and topographical images captured at the last degradation time point demonstrate that the blending component was not leached out during the period of study. The hydrolytic stability of degradable polyester materials can be tailored to obtain different and predetermined degradation profiles for future applications.

SUBMITTER: Arias V

PROVIDER: S-EPMC3892759 | biostudies-literature | 2014 Jan

REPOSITORIES: biostudies-literature

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Tuning the degradation profiles of poly(L-lactide)-based materials through miscibility.

Arias Veluska V Höglund Anders A Odelius Karin K Albertsson Ann-Christine AC

Biomacromolecules 20131206 1

The effective use of biodegradable polymers relies on the ability to control the onset of and time needed for degradation. Preferably, the material properties should be retained throughout the intended time frame, and the material should degrade in a rapid and controlled manner afterward. The degradation profiles of polyester materials were controlled through their miscibility. Systems composed of PLLA blended with poly[(R,S)-3-hydroxybutyrate] (a-PHB) and polypropylene adipate (PPA) with variou ...[more]

PMID: 24279455

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Project description:This methodology permits to simulate the performance of different Poly(D,L-lactide-co-glycolide) copolymer formulations (PDLGA) in the human body, to identify the more influencing variables on hydrolytic degradation and, thus, to estimate biopolymer degradation level. The PDLGA characteristic degradation trends, caused by hydrolysis processes, have been studied to define their future biomedical applications as dental scaffolds. For this purpose, the mass loss, pH, glass transition temperature (Tg) and absorbed water mass of the different biopolymers have been obtained from samples into a phosphate-buffered saline solution (PBS) with initial pH of 7.4, at 37°C (human body conditions). The mass loss has been defined as the variable that characterize the biopolymer degradation level. Its dependence relationship with respect to time, pH and biopolymer formulation has been modelled using statistical learning tools. Namely, generalized additive models (GAM) and nonlinear mixed-effects regression with logistic and asymptotic functions have been applied. GAM model provides information about the relevant variables and the parametric functions that relate mass loss, pH and time. Mixed effects are introduced to model and estimate the degradation properties, and to compare the PDLGA biopolymer populations. The degradation path for each polymer formulation has been estimated and compared with respect to the others for helping to use the proper polymer for each specific medical application, performing selection criteria. It was found that the mass loss differences in PDLGA copolymers are strongly related with the way the pH decay versus time, due to carboxylic acid groups formation. This may occur in those environments in which the degradation products remain relatively confined with the non degraded mass. This is the case emulated with the present experimental procedure. The results show that PDLGA polymers degradation degree, in terms of half life and degradation rate, is increasing when acid termination is included, when DL-lactide molar ratio is reduced, decreasing the midpoint viscosity, or when glycolide is not included.

Dataset Information

Tuning the degradation profiles of poly(L-lactide)-based materials through miscibility.

Publications

Tuning the degradation profiles of poly(L-lactide)-based materials through miscibility.

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