Classical, Coarse-Grained, and Reactive Molecular Dynamics Simulations on Polymer Nanocomposites

Abstract

Polymer-based nanocomposites have been one of the most spotlighted multifunctional condensed materials with the rapidly growing advancement of nanotechnology. Owing to the successful synthesis, manufacture, and characterization of various low-dimensional organic/inorganic nanoparticles and nanocarbon materials, it was expected that unprecedented excellent properties of composites can be achieved. However, disappointing results of the properties of newly designed nanocomposites, yet revealed structure-to-property relationship, and the limitations of the existing theoretical predictive models led to the exploration of new in silico simulation and review of micromechanics models. From the early 2000s, molecular dynamics (MD) simulation studies revealed the physics behind the unpredictable properties and microstructural evolution, such as the size-dependent properties, polymer sheathing, intrinsically weak adhesion between nanocarbon and polymer, and dispersion and agglomeration of fillers. The comprehension of the importance and impact of interface and interphase zone in nanocomposites enabled by the application of MD simulation led to revisiting composite micromechanics and the development of “interface/interphase models.” In this review, the history of the successful application of classical, coarse-grained, and recent reactive MD simulations to the multifunctional properties of nanocomposites is retraced.