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Molecular dynamics simulations of four bioactive silicate glasses containing between 0 (P0) and 12 (P12) mol % P2O5 have been carried out in order to elucidate the structural role of phosphorus in these materials. In particular, we have focused on structural features which can have a direct role in the bioactive mechanism of dissolution and bone bonding. The higher affinity of modifier Na and Ca cations for coordinating phosphate rather than silicate, together with the formation of P-O-Si linkages, lead to increasing repolymerization of the silicate network with increasing P2O5 content, which in principle would represent a negative effect of P inclusion on the glass bioactivity. However, this effect is counterbalanced by the concomitant increase in the amount of free orthophosphate groups, whose fast release is deemed to enhance the bioactivity. The strong affinity of the orthophosphates for calcium ions leads to a clear tendency toward separation of silicate-rich and phosphate-rich phases for the P12 composition. Although this could reduce the bioactivity in the case of P12, in general, the favorable balance between the effects mentioned above should result in a positive effect of partial Si --> P substitution on the glass bioactivity. 相似文献
74.
West KR Ludlow RF Corbett PT Besenius P Mansfeld FM Cormack PA Sherrington DC Goodman JM Stuart MC Otto S 《Journal of the American Chemical Society》2008,130(33):10834-10835
A simple water-soluble naphthalenedithiol building block is converted quantitatively into a series of octameric [2]-catenanes, composed of two interlocked molecular squares. When this mixture is re-equilibrated in the presence of an adamantyl ammonium guest, the catenanes disassemble into their macrocyclic components that bind the guest with nanomolar affinity in water. 相似文献
75.
Half million and million atom systems of sodium silicate glass have been simulated using classical molecular dynamics, and their structures have been examined. Although the structural features are reasonable for the intended glasses, and have a lower configurational energy than smaller systems, they contain features which are indicative of an effective internal, or configurational, temperature higher than the target temperature. This observation is ascribed to the use of a thermostat which controls only the kinetic energy, or momenta, of the particles, and because of the non-equilibrium nature of the simulations, there is no requirement that the potential, or configurational, energy and kinetic energy be coupled. The use of alternative thermostats is suggested. 相似文献
76.
D. Schumayer S. Cormack B.P. van Zyl J. Farry A. Collin E. Zaremba D.A.W. Hutchinson 《The European Physical Journal D - Atomic, Molecular, Optical and Plasma Physics》2012,66(8):1-7
An analytical approach is proposed to investigate the mechanism of implantation of size selected clusters into graphite, in order to explain the origin of linear variation of measured penetration depth with momentum or energy of incident cluster. In agreement with experimental observations, the cluster experiences, during its penetration, a force which consists in a component proportional with cluster velocity and a constant component. Expressions of these forces were obtained in the frame work of this approach. Regardless of whether the cluster breaks down into single atoms on the surface or not, there is evidence for existence of a wave generated under impact of cluster on the surface. Under the assumption that the cluster does not break up at impact on the surface, the penetration depth depends on the cross-section between the cluster and the surface, the cluster velocity and the properties of graphite. When the cluster fragments upon the impact on the surface, the generated wave is followed by a collective motion (??collective cascade??) of displaced atoms of target, including the constituents of cluster themselves, due to the transfer of cluster momentum. Thus, it is these displaced atoms which penetrate in the medium. During this collective penetration, some constituents of cluster can reach a certain depth which may be considered as the range of the deepest implanted constituents of cluster. It is shown that, the depth of penetration depends on the initial radius of cluster, its velocity and the properties of graphite. In addition, the depth varies non linearly with cluster velocity, for small clusters (n ?? 7), while for large clusters (n ?? 13), it varies (i) linearly with cluster velocity (or momentum) when the force proportional with speed of cluster is dominant. (ii) Linearly with the square of cluster velocity (or energy) if the constant force becomes dominant. It is shown that, a mechanism based on a collective motion of displaced atoms including the constituents of cluster themselves, induced by transfer of cluster momentum to the medium, permits to explain the behavior of measured depth of implanted clusters into graphite. This collective motion involves only one free parameter for all clusters of the same nature which are used as projectiles in the same experiment. 相似文献