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Thermal interface materials (TIMs) are extensively used in electronic devices as efficient heat transfer materials. We fabricated all-carbon TIMs by hybridizing single-wall carbon nanotubes (SWCNTs) with graphite and demonstrated their performance by applying them to a thermoelectric generator (TEG) device. The hybrid carbon TIM exhibited maximum thermal conductivity when the SWCNT content was near 10 wt%. The TIM thermal contact resistance measured by a home-made calorimeter setup was 2.19 × 10 −4  m 2 K/W, which did not vary with temperature but decreased with applied pressure. Post-treatment of the TIM with a silane coupling agent further reduced the TIM thermal contact resistance by 30%. When the TIM was placed between a TEG device and a copper heat reservoir, the TEG output power increased with the temperature difference across the TEG and applied pressure. Moreover, the post-treatment of the TIM enhanced the output power of the TEG device by up to 18.5%. This work provides a simple and effective pathway towards a carbon-based TIM that can be applied to a high temperature TEG.

Hybrid carbon thermal interface materials for thermoelectric generator devices