Biphasic calcium phosphate bioceramics composed of hydroxyapatite (HA) and β-tricalcium phosphate (β-TCP) have relevant properties as synthetic bone grafts, such as tunable resorption, bioactivity, and intrinsic osteoinduction. However, they have some limitations associated to their condition of high-temperature ceramics. In this work self-setting Biphasic Calcium Phosphate Cements (BCPCs) with different HA/β-TCP ratios were obtained from self-setting α-TCP/β-TCP pastes. The strategy used allowed synthesizing BCPCs with modulated composition, compressive strength, and specific surface area. Due to its higher solubility, α-TCP was fully hydrolyzed to a calcium-deficient HA (CDHA), whereas β-TCP remained unreacted and completely embedded in the CDHA matrix. Increasing amounts of the non-reacting β-TCP phase resulted in a linear decrease of the compressive strength, in association to the decreasing amount of precipitated HA crystals, which are responsible for the mechanical consolidation of apatitic cements. Ca2+ release and degradation in acidic medium was similar in all the BCPCs within the timeframe studied, although differences might be expected in longer term studies once β-TCP, the more soluble phase was exposed to the surrounding media.
Calcium Phosphates (CaPs) have excellent bone regeneration capacity, and their combination with specific drugs is of interest because it allows adding new functionalities. In CaPs, drug release is mainly driven by diffusion, which is strongly affected by the porosity of the matrix and the drug-material interaction. Therefore, it is very difficult to tune their drug release properties beyond their intrinsic properties. Furthermore, when the CaPs are designed as scaffolds, the increased complexity of the macrostructure further complicates the issue.; This work investigates for the first time the use of biocompatible plasma-polymers to provide a tool to control drug release from drug-loaded CaP scaffolds with complex surfaces and intricate 3D structure. Two different CaPs were selected displaying great differences in microstructure: low-temperature CaPs (Calcium-deficient hydroxyapatite cements, CDHA) and sintered CaP ceramics (beta-Tricalcium Phosphate, beta-TCP). The deposition of PCL-co-PEG (1: 4) copolymers on CaPs was achieved by a low pressure plasma process, which allowed coating the inner regions of the scaffolds up to a certain depth. The coating covered the micro and nanopores of the CaPs surface and produced complex geometries presenting a nano and micro rough morphology which lead to low wettability despite the hydrophilicity of the copolymer. Plasma coating with PCL-co-PEG on scaffolds loaded with Simvastatin acid (potentially osteogenic and angiogenic) allowed delaying and modulating the drug release from the bone scaffolds depending on the thickness of the layer deposited, which, in turn depends on the initial specific surface area of the CaP. (C) 2016 Elsevier Ltd. All rights reserved.Peer ReviewedPostprint (author's final draft
Calcium phosphate cements (CPCs) are extensively used as synthetic bone grafts, but their poor toughness limits their use to nonload-bearing applications. Reinforcement through introduction of fibers and yarns has been evaluated in various studies but always resulted in a decrease in elastic modulus or bending strength when compared to the CPC matrix. The aim of the present work was to improve the interfacial adhesion between fibers and matrix to obtain tougher biocompatible fiberreinforced calcium phosphate cements (FRCPCs). This was done by adding a polymer solution to the matrix, with chemical affinity to the reinforcing chitosan fibers, namely trimethyl chitosan (TMC). The improved wettability and chemical affinity of the chitosan fibers with the TMC in the liquid phase led to an enhancement of the interfacial adhesion. This resulted in an increase of the work of fracture (several hundred-fold increase), while the elastic modulus and bending strength were maintained similar to the materials without additives. Additionally the TMC-modified CPCs showed suitable biocompatibility with an osteoblastic cell line. Graphical Abstract (for review) Highlights HIGHLIGHTS• Calcium phosphate cements were reinforced with chitosan fibers and soluble chitosan• The chemical affinity of fibers and matrix improved interfacial adhesion• Mechanical reinforcement was achieved thanks to a good fiber-matrix adhesion• Fiber-reinforced cements were significantly tougher than non-reinforced analogues • The modified cement matrix supported osteoblast proliferation 1 2 3 4 5 6 7 8 9 10 11 12 13 14 15 16 17 18 19 20 21 22 23 24 25 26 27 28 29 30 31 32 33 34 35 36 37 38 39 40 41 42 43 44 45 46 47 48 49 50 51 52 53 54 55 56 57 58 59 60 61 62 63 64 65 -2 - AbstractCalcium phosphate cements (CPCs) are extensively used as synthetic bone grafts, but their poor toughness limits their use to non-load-bearing applications. Reinforcement through introduction of fibers and yarns has been evaluated in various studies but always resulted in a decrease in elastic modulus or bending strength when compared to the CPC matrix. The aim of the present work was to improve the interfacial adhesion between fibers and matrix to obtain tougher biocompatible fiber-reinforced calcium phosphate cements (FRCPCs). This was done by adding a polymer solution to the matrix, with chemical affinity to the reinforcing chitosan fibers, namely trimethyl chitosan (TMC). The improved wettability and chemical affinity of the chitosan fibers with the TMC in the liquid phase led to an enhancement of the interfacial adhesion. This resulted in an increase of the work of fracture (several hundred-fold increase), while the elastic modulus and bending strength were maintained similar to the materials without additives. Additionally the TMC-modified CPCs showed suitable biocompatibility with an osteoblastic cell line.
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