Thermal interface materials (TIMs) are widely used as gap–filler materials between electronic devices such as LEDs and ICs and their heat sink and aim to control the heat dissipation and to provide mechanical anchoring. As the rated power densities of electronic devices are increasing rapidly, the TIMS are exposed to higher thermal and mechanical loads. The resulting aging of the TIMs may lead to delamination and internal crack formation causing loss of heat transfer as well as mechanical integrity leading to premature device failure. Therefore there is an increased demand for efficient and reliable TIM which can avoid, or even better, mitigate this thermomechanical damage. This thesis aims to contribute to the introduction of self–healing concepts into polymer–based TIMs to increase their reliability and service lifetime. As such, each chapter targets one of the scientific issues that are related to the development of commercial self–healing TIMs.@en

In the present work we show the effect of graphene loading on the restoration of the mechanical properties and thermal and electrical conductivity of a self-healing natural rubber nanocomposite. The graphene loading led to a minimal enhancement of mechanical properties and yielded a modest increase in thermal and electrical conduction. The polymer nanocomposites were macroscopically damaged (cut) and thermally healed for 7 h in a healing cell. Different healing trends as function of the graphene content were found for each of the functionalities: (i) thermal conductivity was fully restored independently of the graphene filler loading; (ii) electrical conductivity was only restored to a high degree above the percolation threshold; and (iii) tensile strength restoration increased more or less linearly with graphene content but was never complete. A dedicated molecular dynamics analysis by dielectric spectroscopy of the pristine and healed samples highlighted the role of graphene-polymer interactions at the healed interphase on the overall restoration of the different functionalities. Based on these results it is suggested that the dependence of the various healing efficiencies with graphene content is due to a combination of the graphene induced lower crosslinking density, as well as the presence of strong polymer-graphene interactions at the healed interphase.@en

Thermal interface materials (TIMs) are widely used in all kinds of electronic devices to handle the heat dissipation and the mechanical anchoring of the heat producing component. The aging of TIMs may lead to delamination and internal crack formation causing a loss of heat transfer and mechanical integrity both leading to premature device failure. In the present work, a novel TIM system based on a self-healing organic-inorganic polymer matrix filled with spherical glass beads is presented which is capable of healing both the thermal conductivity and the mechanical properties upon thermal activation. The effect of particle volume concentration (PVC) and particle size on tensile strength and thermal conductivity healing behavior is investigated. The results show that a higher PVC increases the mechanical property but decreases mechanical healing. For the same PVC, bigger particles lead to lower mechanical properties but higher thermal conductivities and higher mechanical healing efficiencies.

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