Abstract

Dual setting cements composed of an in situ forming hydrogel and a reactive mineral phase combine high compressive strength of the cement with sufficient ductility and bending strength of the polymeric network. Previous studies were focused on the modification with non-degradable hydrogels based on 2-hydroxyethyl methacrylate (HEMA). Here, we describe the synthesis of suitable triblock degradable poly(ethylene glycol)-poly(lactide) (PEG-PLLA) cross-linker to improve the resorption capacity of such composites. A study with four different formulations was established. As reference, pure hydroxyapatite (HA) cements and composites with 40 wt% HEMA in the liquid cement phase were produced. Furthermore, HEMA was modified with 10 wt% of PEG-PLLA cross-linker or a test series containing only 25% cross-linker was chosen for composites with a fully degradable polymeric phase. Hence, we developed suitable systems with increased elasticity and 5–6 times higher toughness values in comparison to pure inorganic cement matrix. Furthermore, conversion rate from α-tricalcium phosphate (α-TCP) to HA was still about 90% for all composite formulations, whereas crystal size decreased. Based on this material development and advancement for a dual setting system, we managed to overcome the drawback of brittleness for pure calcium phosphate cements.

Highlights

  • Bone is often described as natural miracle due to its impressive mechanical properties

  • It has a very high load-capacity of ~90–190 MPa [1] for cortical bone, while at the same time it provides elastic and ductile properties with a high fracture resistance. This high stability is based on its structural composition, as natural bone is a composite mainly consisting of apatite, collagen, and water [2,3]. This leads to the idea to mimic bone structure in synthetic materials by combining an inorganic phase based on calcium phosphate cements (CPCs) with an organic polymeric matrix

  • H40P10 and P25, that were produced with the synthesized monomer, resulted in an even faster setting that only took halve of the time than the formulation with 40 wt% hydroxyethyl methacrylate (HEMA) (H40) alone

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Summary

Introduction

Bone is often described as natural miracle due to its impressive mechanical properties. It has a very high load-capacity of ~90–190 MPa [1] for cortical bone, while at the same time it provides elastic and ductile properties with a high fracture resistance This high stability is based on its structural composition, as natural bone is a composite mainly consisting of apatite, collagen, and water [2,3]. According to the chosen pH-values during setting reaction as well as different solubility products constants Ksp , one can distinguish between brushite (DCPD, CaHPO4 ·2H2 O; pH ≤ ~4.2) and hydroxyapatite (HA, Ca5 (PO4 ) OH; pH ≥ ~4.2) forming cements The latter one is clinically a very well established system due to its outstanding properties like bioactivity, osteoconductivity [5] and stochiometric similarity to mineral components present in bone and teeth [6]. Bohner [7] describes an “excellent”

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