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

WF Zhang and ZM Hu and YL Lu and TH Zhou and H Zhang and XY Zhao and L Liu and LQ Zhang and YY Gao, JOURNAL OF PHYSICAL CHEMISTRY B, 127, 10243-10251 (2023).

DOI: 10.1021/acs.jpcb.3c06476

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 cross-linking 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.

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