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The effects of molecular structure on the mechanical properties of a polymer system has long been of interest to polymer chemists, physicists, and engineers. Much work has been done in mechanical modeling and in statistical mechanics to describe the working polymer. With the advent of molecular mechanics and dynamics and the general use of Newtonian techniques, an added dimension is available to study structural effects on the inter- and intramolecular level that may directly contribute to mechanical behavior. In this study, molecular modeling has been used in order to understand the water absorption characteristics of polybenzimidazole (PBI) and its effect on mechanical properties.... Polybenzimidazole, Molecular modeling, Structure-property correlations, Mechanical behavior, Water affinity, Hydrogen bonding tendencies.