Polymer/Carbon Composites with Versatile Interfacial Interactions for High Performance Carbon‐Based Thermoelectrics: Principles and Applications

Abstract The urgent demand for renewable energy has attracted widespread interest in polymer‐based thermoelectric materials due to easy fabrication, high flexibility, low toxicity, low thermal conductivity, and great potential in industrial applications. However, the power factors of the polymers are still quite low compared with those of their inorganic counterparts, resulting in a low energy conversion efficiency. Highly conductive carbon materials, including graphene and carbon nanotubes, have recently been incorporated into the polymer matrix through intrinsic chemical intimacy, providing new opportunities to tune the thermoelectric properties. In particular, the characteristic π‐π coupling and other interactions between the two components have contributed to unique mechanisms for better thermoelectric performance beyond the simple rule of mixtures. This paper aims to review the up‐to‐date progress in polymer/carbon nanocomposites along with various compositions and novel synthetic strategies. The salient aspects of this review are characteristic interactions and various mechanisms, which might result in enhanced thermoelectric properties and subsequent potential applications in energy harvesting, wearable electronics, photo‐thermoelectrics, and other devices.