Molecular Dynamics Simulation on the Heat Transfer in the Cross-Linked Poly(dimethylsiloxane)

Abstract

In this work, the effect of cross-linking degree and stretching on the thermal conductivity of poly(dimethylsiloxane) (PDMS) is explored by performing a molecular dynamics simulation. Our results demonstrate that the thermal conductivity of PDMS exhibits a monotonous rise with an increase in the crosslinking degree. By decomposing the total heat flux into three microscopic heat transfer modes, the high cross-linking degree improves the contribution from bonding interactions to the heat transfer more than that from the nonbonding interactions. An analysis of the vibrational density of states shows a blue-shift of the vibrational modes at low frequencies, indicating a large phonon group velocity due to the strong interchain bonding interaction. From the spectral distribution of heat flux, the spectral contributions are shifted toward the higher frequencies with the increasing cross-linking degree, which reflects more contribution from the high-frequency modes to the heat transfer. Stretching can improve the thermal conductivity parallel to the tensile direction with the increase in strain. This is mainly due to the further improved contribution of bonding interactions or high-frequency modes to heat transfer. Interestingly, the anisotropy of the thermal conductivity first decreases and then increases with the increasing cross-linking degree. Our study conducts a detailed investigation of the thermal conductivity of cross-linked PDMS, providing guidance on the application of thermal interface materials.

Thermal Conductivity of the Graphene/Polydimethylsiloxane Composite by Manipulating the Network Structure

“…The equilibrium state of the simulation systems is considered to be reached when the energy, temperature, and density are unchanged. The density, mean-squared radius of gyration, and the thermal conductivity of PDMS are comparable between our simulation model and experiments, ,, which can prove that the used parameters are reasonable. Next, the NEMD method is applied to compute the thermal conductivity of composites and the GE–GE ITR under the NVE ensemble.…”

“…A cutoff distance of 1.2 nm is chosen. All the force field parameters can be found in the Tables SI and SII. ,, The adaptive intermolecular reactive empirical bond order (AIREBO) potential is employed to describe the atoms interaction in GE, which is widely used to calculate the carbon-based materials . Moreover, the Lorentz–Berthelot mixing rule is applied to determine the nonbonded interactions between PDMS and GE atoms.…”