Muiltiscale modeling of electrical conductivity of R-BAPB polyimide + carbon nanotubes nanocomposites

TL;DR

This paper presents a multiscale modeling approach combining molecular dynamics, quantum transport calculations, and Monte Carlo simulations to predict the electrical conductivity of R-BAPB polyimide with carbon nanotubes, aligning with experimental data.

Contribution

It introduces a comprehensive multiscale modeling framework that links atomic-scale interactions to macroscopic conductivity in CNT-polymer composites, considering junction geometry and agglomeration effects.

Findings

Contact resistance strongly depends on CNT junction geometry.

Predicted conductivity just above percolation threshold, matching experiments.

Insights into mechanisms for further conductivity reduction.

Abstract

The electrical conductivity of the polyimide R-BAPB polymer filled with single-wall carbon nanotubes (CNT) with chirality (5,5) is modeled using a multi-scale approach. The modeling starts with molecular dynamics simulations of time-dependent fluctuating atomic configurations of polymer filled CNTs junctions. Then the atomic positions obtained in the first step are used to perform fully first-principles microscopic calculations of the CNTs junctions contact resistances using the Green's function based quantum transport technique. And finally, those contact resistances are supplied as an input to a statistical calculation of a CNTs ensemble conductivity using a Monte Carlo percolation model. The results of the first-principles calculations show a very strong dependence of the polymer filled CNTs junctions contact resistance on the geometry of CNTs junctions, including an angle $\varphi$ between nanotubes axes and the positions of polymer atoms around CNTs. Incorporating into the percolation model this strong dependence as well as CNTs agglomeration, pushed the calculated values of electrical conductivity just above the percolation threshold below 0.01 S/m, which is within the experimental range for composites with various base polymers. Possible mechanisms for further reduction of composites conductivity are discussed.