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

Abstract 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.