Charge Trap and Oxygen Barrier Engineering in Voltage-Stabilizing Grafted Silicone Rubber via Multiscale Molecular Simulations

The present theoretical study proposes and unravels chemical graft modification using a novel voltage stabilizer (3-amino-5-chlorophenyl 3-fluorophenyl methanone, ACFM) to ameliorate electrical insulation performance, oxygen-resistant characteristics, and thermal stability of addition-cure silicone rubber (SiR) used for cable accessory insulation in power transmission systems. First-principles calculations demonstrate that chemically grafted ACFM introduces shallow hole and electron traps into addition-cure SiR macromolecules to respectively impede hole transport and restrict hot electron production. Through molecular dynamics and Monte Carlo simulation, the chemically grafted ACFM is verified to enhance chain segment coalescence and decrease oxygen compatibility of addition-cure SiR macromolecules due to its higher dipole moment, leading to a reduction in oxygen permeation and improvement in thermal stability of the SiR crosslinked material. It is indicated from first-principles oxidation reaction paths that chemical grafting ACFM contributes positively to the oxidative stability of addition-cure SiR. The improved abilities of charge trapping and withstanding high temperatures together with enhanced resistance to both oxygen infiltration and oxidation of the addition-cure SiR material, as unraveled on a molecular scale in this research, open an avenue for developing advanced polymer dielectrics applied in harsh environments.