It has already been shown that sono-electrodeposition can be used to coat activated carbon fiber cloth (ACC) with calcium phosphates (CaP) and we recently demonstrated that cathodic polarization at-1 V / Hg/Hg2SO4 was the best parameter to obtain a carbonated calcium deficient hydroxyapatite (CDA) coating with optimal uniformity and homogeneity. In the present study, we investigated whether this technique was suitable to dope this carbonated CDA coating by partial substitution with another bivalent cation such as strontium. We show here that a strontium-substituted carbonated CDA coating can be produced and quantitatively controlled up to at least 10 at.%. In this range we demonstrate that the presence of strontium does not modify either the textural or the structural properties of the carbonated CDA. Owing to the well-known effect of both carbonated CDA and strontium in bone formation, the biocompatibility of ACC coated or not with carbonated CDA or with strontium substituted carbonated CDA was tested using primary human osteoblasts. Our data revealed a positive and dose-dependent effect of strontium addition on osteoblast activity and proliferation. In conclusion, we show here that electrodeposition at-1 V is a suitable and easy process to incorporate cations of biological interest into CaP coating.
We capitalized herein the inherent tortuosity of bicontinuous microemulsion to conceive nanostructured drug-delivery devices. First, we show that it is possible to synthesize bicontinuous materials with continuous hydrophilic domains of the poly(N-isopropylacrylamide) (PNIPAM) network entangled with continuous hydrophobic polymer domains, with dual-phase continuity being imposed by the bicontinuous microemulsions used as a soft template. Particular attention is paid to the microemulsion formulations using a surfmer to preserve the one-to-one replication of the bicontinuous nanostructure after polymerization. These materials keep a volume phase transition with temperature that allows considering them as drug carriers for controlled release. PNIPAM, which plays the role of the active ingredient reservoir, is confined in the bicontinuous structure. As expected, the PNIPAM enclosure limits the surface area in contact with the releasing aqueous solution and thus slows down the desorption of aspirin, which is used as a model drug. The hydrophobic polymers play the role of in situ-created transport barriers without hindering it as all the loaded aspirin in this bicontinuous structure still remains available.
Calcium phosphate and derivatives have been known for decades as bone compatible biomaterials. In this work, the chemical composition, microtexture, and structure of calcium phosphate deposits on carbon cloths were investigated. Three main types of deposits, obtained through variation of current density in using the sono-electrodeposition technique, were elaborated. At low current densities, the deposit consists in a biomimetic, plate-like, carbonated calcium-deficient hydroxyapatite (CDA), likely resulting from the in situ hydrolysis of plate-like octacalcium phosphate (OCP), while at higher current densities the synthesis leads to a needle-like carbonated CDA. At intermediate current densities, a mixture of plate-like and needle-like carbonated CDA is deposited. This established that sono-electrodeposition is a versatile process that allows the coating of the carbon scaffold with biomimetic calcium phosphate while tuning the morphology and chemical composition of the deposited particles, thereby bringing new insights in the development of new biomaterials for bone repair.
A biomaterial that is both bioactive and capable of controlled drug release is highly attractive for bone regeneration. In previous works, we demonstrated the possibility of combining activated carbon fiber cloth (ACC) and biomimetic apatite (such as calcium-deficient hydroxyapatite (CDA)) to develop an efficient material for bone regeneration. The aim to use the adsorption properties of an activated carbon/biomimetic apatite composite to synthetize a biomaterial to be used as a controlled drug release system after implantation. The adsorption and desorption of tetracycline and aspirin were first investigated in the ACC and CDA components and then on ACC/CDA composite. The results showed that drug adsorption and release are dependent on the adsorbent material and the drug polarity/hydrophilicity, leading to two distinct modes of drug adsorption and release. Consequently, a double adsorption approach was successfully performed, leading to a multifunctional and innovative ACC-aspirin/CDA-tetracycline implantable biomaterial. In a second step, in vitro tests emphasized a better affinity of the drug (tetracycline or aspirin)-loaded ACC/CDA materials towards human primary osteoblast viability and proliferation. Then, in vivo experiments on a large cortical bone defect in rats was carried out to test biocompatibility and bone regeneration ability. Data clearly highlighted a significant acceleration of bone reconstruction in the presence of the ACC/CDA patch. The ability of the aspirin-loaded ACC/CDA material to release the drug in situ for improving bone healing was also underlined, as a proof of concept. This work highlights the possibility of bone patches with controlled (multi)drug release features being used for bone tissue repair.
We have previously shown that activated carbon fiber cloth (ACC) either uncoated or coated with carbonated calcium-deficient hydroxyapatite (CDA), namely ACC and ACC/CDA, were biocompatible in vitro with human osteoblasts. Here we hypothesized that ACC and ACC/CDA could be used as tissue patches in vivo to accelerate wounded bone healing. In a model of rat femoral defect, we have compared spontaneous cortical bone regeneration with regeneration in the presence of ACC and ACC/CDA patches. At day 7, 14 and 21, bone formation was evaluated using micro computed tomography (µCT), magnetic resonance imaging (MRI) and histological analysis. Our results demonstrate first that these ACC tissues are highly biocompatible in vivo, and second that ACC/CDA patches apposition results in the acceleration of bone reconstruction due to a guiding action of the ACC fibers and an osteogenic effect of the CDA phase. We guess that this approach may represent a valuable strategy to accelerate bone regeneration in human.
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