Thermal interface materials (TIMs) are one of the efficacious ways to alleviate the heat accumulation problem of microelectronics devices. However, conventional TIMs based on polydimethylsiloxane (PDMS) always suffer from mechanical damage, leading to shortened service life or loss of thermal conductivity. In this work, we fabricated a high-thermal conductivity and fast self-healable Al2O3@siloxane composite by hydrosilylation reaction. The siloxane matrix consisted of thermosetting silicone rubber matrix (SR) and heat reversibility matrix (SCNR); the SR was synthesized via hydrosilylation between silicon hydrogen bond and vinyl, the SCNR was fabricated by thermal-curing between amino and carboxyl functionalized PDMS. Different sized spherical Al2O3 fillers were introduced into the SR/SCNR matrix system to construct the Al2O3@SR/SCNR composites. By adjusting the ratio of SR/SCNR, the obtained composites can achieve flexibility, self-healing and high filling simultaneously. It is notable that the self-healing efficiency of the composite is high, up to 95.6% within 3 minutes with 6.7 wt% mass ratio of SCNR/SR; these fast self-healing behaviors benefit from the assistance of thermal diffusion by 3D heat conduction pathways on the rearrangement of the dynamic cross-linked network. The resultant composites also exhibited the optimal thermal conductivity of 5.85 W mK-1. This work provides a novel approach for constructing longer service life and high thermal conductivity multifunctional TIM based PDMS.
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