▎ 摘　　要

Thermal interface material (TIM) plays a key role in dissipating the huge volume of heat energy produced by the high-density electronic circuits nowadays. Because of the excellent thermal transport performance of graphene, composites composed of polymer matrices and graphene fillers have been anticipated to perform as excellent TIMs. However, until now the thermal conductivity achieved on these polymer-graphene composite TIMs are not as expected. Firstly, the effective heat transfer performance of the TIMs is limited by the large thermal boundary resistance existing at the interfaces between polymeric matrices and graphene. Secondly, strong interfacial binding between matrices and fillers is critical to the performance of composite TIMs, and the interfacial binding behavior between polymers and graphene is still to be revealed. By using molecular dynamics simulations, this research deals with modulating the thermal boundary resistance and interfacial binding behavior between epoxy and graphene. The results show that treating the graphene with covalent grafts or non-covalent molecular interposers could lower the thermal boundary resistance at the interface between epoxy and graphene. The interfacial binding between epoxy and graphene is strengthened by treating the graphene with covalent grafts, while not by adding noncovalent molecular interposers. The findings herein offer valuable guidance for the development of highly effective TIMs based on graphene.