The improved thermal conductivity and heat dissipation capacity of elastomer-based thermal interface materials through promoting the surface interactions and complete networks

Polymer-based thermal interface materials (TIMs) with excellent thermal conductivity and heat dissipation capabilities play a crucial role in addressing the issue of heat accumulation in advanced integrated electronics. However, establishing improved surface interactions and complete networks to enhance efficient phonon transfer remains a significant challenge. To tackle this problem, surface modification and ice-templating techniques are commonly employed to create the robust interface crosslinks and continuously thermal conductive pathways. Herein, 2-mercaptobenzimidazole (MB) was used as a reducing and modifying agent to functionalize graphene oxide (rGO-MB) within the three-dimensional networks, which was prepared using a combination of hydrothermal and ice-templating methods. As a result, the reduced graphene oxide/natural rubber (rGO-MB/NR) TIMs exhibited a remarkable through-plane thermal conductivity of 0.93 W m −1 K −1 with a filler loading of 3 wt%. The enhanced interface interactions between rGO-MB and NR, combined with the establishment of a three-dimensional network, significantly contributed to the improved thermal conductivity and heat dissipation capabilities. Moreover, the obtained TIMs demonstrated favorable mechanical properties (5.06 MPa, 502%) and excellent insulation performance (3 × 10 13 Ω cm). These findings provide the valuable insights into potential solutions for mitigating heat accumulation issues in next-generation electronics. Highlights rGO-MB with thiol groups was obtained by the hydrothermal method. Interactions between rGO-MB and NR mainly depended on the chemical bonds. rGO-MB/NR TIMs owned the improved thermal management performance.