Influence of crystallization conditions on the tensile properties of radiation crosslinked, vitamin E stabilized UHMWPE.

Radiation crosslinking for ultra-high molecular weight polyethylene results in improved wear resistance but a reduction in mechanical properties. Incorporation of vitamin E has been known to decrease the rate of oxidative degradation occurring through radiation crosslinking and prevents the need for post-irradiation melting with subsequent loss of crystallinity. In this study, we aimed to determine the effect of thermal treatments prior to crosslinking on the morphology and tensile properties of vitamin-E-containing polyethylene. Vitamin-E-blended polyethylene was melted and subsequently quenched in ice water in order to induce high rate crystallization. A second group was additionally annealed at 126°C following quenching and all samples were irradiated using electron beam radiation to a dose of 100kGy. The morphology of control, quenched and quench-annealed polyethylene was characterized using small angle x-ray scattering and differential scanning calorimetry. Tensile properties of these polyethylenes were measured before and after radiation crosslinking with equilibrium swelling experiments performed to assess the crosslink density of irradiated samples. This study shows how the tensile properties of polyethylene can be enhanced by varying thermal treatments prior to crosslinking; and thus how it may be possible to offset the reduction in tensile properties afforded by the crosslinking process.

Characterization of network parameters for UHMWPE by plane strain compression.

Ultra-high molecular weight polyethylene (PE) is used as a bearing material for total joint replacement prostheses since it is a tough, wear-resistant semicrystalline polymer. Despite its high resistance to wear, PE components have shown measureable wear in vivo, which can cause wear-particle induced osteolysis. Crosslinking of PE using ionizing radiation has been shown to increase wear resistance since both chemical crosslinks and physical entanglements provide high resistance to wear. Molecular characterization of crosslinked PEs is usually conducted using equilibrium swelling or by quantifying gel content. In this study, we compared crosslink densities and molecular weight between crosslinks derived from equilibrium swelling to those obtained by applying the Gaussian and Eight-Chain model to describe plane strain compression of the PE melt. The latter approach has the advantage of accounting for contributions of entanglements to the overall crosslink density, which solvent-based techniques largely neglect. As expected, the crosslink density calculated from model fitting increased monotonically with increase in radiation dose in a 0-200kGy dose range, with a corresponding monotonic decrease in molecular weight between crosslinks, but provided higher values of crosslink density and correspondingly lower values of molecular weight between crosslinks compared to the equilibrium swelling technique.

The effects of degree of crosslinking on the fatigue crack initiation and propagation resistance of orthopedic-grade polyethylene.

Crosslinked ultrahigh molecular weight polyethylene (UHMWPE) has been recently approved by the Food and Drug Administration for use in orthopedic implants. The majority of commercially available UHMWPE orthopedic components are crosslinked using e-beam or gamma radiation. The level of crosslinking is controlled with radiation dose and free radicals are eliminated through heat treatments to prevent long-term degradation associated with chain scission or oxidation mechanisms. Laboratory studies have demonstrated a substantial improvement in the wear resistance of crosslinked UHMWPE. However, a concern about the resistance to fatigue damage remains in the clinical community, especially for tibial components that sustain high cyclic contact stresses. The objective of this study was to investigate both the initiation and propagation aspects of fatigue cracks in radiation crosslinked medical-grade UHMWPE. This work evaluated three levels of radiation, which induced three crosslink densities, on the fatigue crack propagation and total fatigue life behavior. Both as-received UHMWPE, as well as those that underwent an identical thermal history as the crosslinked UHMWPE were used as controls. Fractured crack propagation specimens were examined using scanning electron microscopy to elucidate fatigue fracture mechanisms. The results of this work indicated that a low crosslink density may optimize the fatigue resistance from both a crack initiation and propagation standpoint.

J-integral fracture toughness and tearing modulus measurement of radiation cross-linked UHMWPE.

Radiation and chemical cross-linking of medical grade ultrahigh molecular weight polyethylene (UHMWPE) has recently been utilized in an effort to improve wear performance of total joint replacement components. However, reductions in mechanical properties with cross-linking are cause for concern regarding the use of cross-linked UHMWPE for high-stress applications such as in total knee replacement prostheses. In this study, the fracture behavior of radiation cross-linked UHMWPE was compared to that of uncross-linked UHMWPE. The Rice and Sorensen model that utilizes mechanical parameters obtained from uniaxial tensile and compact tension tests was used to calculate the steady state J-integral fracture toughness, Jss, for radiation cross-linked UHMWPE. Jss decreased monotonically with increase in radiation dose. UHMWPE exhibited tough, ductile tearing behavior with stable crack growth when it was cross-linked using a gamma radiation dose of 0-50 kGy. However, in cross-linked UHMWPE irradiated to a dose of 100 and 200 kGy, unstable fracture occurred spontaneously upon attaining the initial crack driving force, J1c. This indicates that a high degree of cross-linking is less desirable for high-stress applications in orthopaedic implants. However, a substantial increase in J1c, even at a low degree of cross-linking, suggests that a low degree of cross-linking may be beneficial for resistance to delamination and catastrophic failure, both of which require an initiation step for the fracture to propagate in the material. This mechanical test should, however, be considered along with fatigue tests and joint simulator testing before determination of an appropriate amount of cross-linking for total joint replacement prostheses that experience high stresses.

Morphology of rod stock and compression-moulded sheets of ultra-high-molecular-weight polyethylene used in orthopaedic implants.

Compression-moulded sheets and extruded rods of ultra-high-molecular-weight polyethylene (UHMWPE) are currently used in the production of joint replacement prostheses. Crystallographic texture present in rods and sheets of UHMWPE was measured using a combination of small-angle X-ray scattering and wide-angle X-ray diffraction. Crystallographic texture can induce anisotropy in macroscopic properties of polymers, such as modulus and yield stress. Both rods and sheets of UHMWPE revealed a low but discernible degree of preferred orientation of polyethylene chains within crystallites. There was a spatial variation in crystallographic orientation in extruded rods. The direction of chain alignment within crystallites located near the outer surface of rods was orthogonal to the radial direction, whereas the chain direction was orthogonal to the axial or extrusion direction in crystallites located near the centreline of extruded rods. Crystallographic texture was spatially uniform in compression-moulded sheets with the chain direction within crystallites aligned orthogonal to the moulding direction. In both cases the induced crystallographic texture can be explained in terms of crystallization from an oriented melt.