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Combinatorial Design of Hydrolytically Degradable, Bone-like Biocomposites Based on PHEMA and Hydroxyapatite.

ABSTRACT: With advantages such as design flexibility in modifying degradation, surface chemistry, and topography, synthetic bone-graft substitutes are increasingly demanded in orthopedic tissue engineering to meet various requirements in the growing numbers of cases of skeletal impairment worldwide. Using a combinatorial approach, we developed a series of biocompatible, hydrolytically degradable, elastomeric, bone-like biocomposites, comprising 60 wt% poly(2-hydroxyethyl methacrylate-co-methacrylic acid), poly(HEMA-co-MA), and 40 wt% bioceramic hydroxyapatite (HA). Hydrolytic degradation of the biocomposites is rendered by a degradable macromer/crosslinker, dimethacrylated poly(lactide-b-ethylene glycol-b-lactide), which first degrades to break up 3-D hydrogel networks, followed by dissolution of linear pHEMA macromolecules and bioceramic particles. Swelling and degradation were examined at Hank's balanced salt solution at 37 °C in a 12-week period of time. The degradation is strongly modulated by altering the concentration of the co-monomer of methacrylic acid and of the macromer, and chain length/molecular weight of the macromer. 95% weight loss in mass is achieved after degradation for 12 weeks in a composition consisting of HEMA/MA/Macromer = 0/60/40, while 90% weight loss is seen after degradation only for 4 weeks in a composition composed of HEMA/MA/Macromer = 27/13/60 using a longer chain macromer. For compositions without a co-monomer, only about 14% is achieved in weight loss after 12-week degradation. These novel biomaterials offer numerous possibilities as drug delivery carriers and bone grafts particularly for low and medium load-bearing applications.

SUBMITTER: Huang J

PROVIDER: S-EPMC3601847 | biostudies-literature | 2013 Jan

REPOSITORIES: biostudies-literature

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Combinatorial Design of Hydrolytically Degradable, Bone-like Biocomposites Based on PHEMA and Hydroxyapatite.

Huang Jijun J Zhao Dacheng D Dangaria Smit J SJ Luan Xianghong X Diekwisch Thomas G H TG Jiang Guoqing G Saiz Eduardo E Liu Gao G Tomsia Antoni P AP

Polymer 20121213 2

With advantages such as design flexibility in modifying degradation, surface chemistry, and topography, synthetic bone-graft substitutes are increasingly demanded in orthopedic tissue engineering to meet various requirements in the growing numbers of cases of skeletal impairment worldwide. Using a combinatorial approach, we developed a series of biocompatible, hydrolytically degradable, elastomeric, bone-like biocomposites, comprising 60 wt% poly(2-hydroxyethyl methacrylate-<i>co</i>-methacrylic ...[more]

PMID: 23525786

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Project description:Poly(lactic acid) choline iodide ester methacrylate, poly(PLA4ChMA), is a cationic degradable polymer that can flocculate particles and dewater oil sands from tailings ponds. This novel material has yet to be characterized in terms of environmental and human health. If ingested, this substance may become bioaccessible. The bioaccessibility (bioaccessible fraction) of an ingested contaminant is a measure of the portion of an ingested dose that solubilizes and may be available for systemic absorption. In the present study, the partially degraded flocculant and its degradation products, modelled using lactic acid and choline chloride, were subjected to a modified physiologically based extraction test (PBET). Bioaccessible fractions were estimated by proton nuclear magnetic resonance (1H-NMR) spectroscopy and by high-performance liquid chromatography (HPLC). The measured bioaccessibility of lactic acid in gastric solution containing choline chloride is ∼100% but slightly dropped to 94% in intestinal solution at a solid-to-liquid ratio of 1:200. The partially degraded poly(PLA4ChMA) did not degrade further during the PBET and is not solubilized (i.e., 0% bioaccessibility) in the gastric phase but is fully solubilized (i.e., 100% bioaccessibility) in the intestinal phase. At the end of PBET intestinal digestion, the molar ratio of lactic acid to choline chloride in the presence of degraded poly(PLA4ChMA) was 2, approximately the same as in the initial solution. Thus, lactic acid and choline chloride are solubilized to the same extents in both gastric and intestinal solutions. Results suggest that HPLC can be used to directly estimate the bioaccessibility of lactic acid, whereas 1H - NMR may be used to indirectly quantify the bioaccessibility of both lactic acid and choline chloride by determining their molar ratio in PBET extracts. In future works, these findings may be applied to the estimation of risks from exposure to poly(PLA4ChMA) as well as to the remediation of contaminants flocculated by poly(PLA4ChMA) in tailings ponds and in other wastewaters.

Dataset Information

Combinatorial Design of Hydrolytically Degradable, Bone-like Biocomposites Based on PHEMA and Hydroxyapatite.

Publications

Combinatorial Design of Hydrolytically Degradable, Bone-like Biocomposites Based on PHEMA and Hydroxyapatite.

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