Significantly Enhanced Thermoelectric Performance of Graphene through Atomic-Scale Defect Engineering via Mobile Hot-Wire Chemical Vapor Deposition Systems.

Over the years, numerous studies have attempted to develop two-dimensional (2D) materials for improving both the applicability and performance of thermoelectric devices. Among the 2D materials, graphene is one of the promising candidates for thermoelectric materials owing to its extraordinary electrical properties, flexibility, and nontoxicity. However, graphene synthesized through traditional methods suffers from a low Seebeck coefficient and high thermal conductivity, resulting in an extremely low thermoelectric figure of merit (ZT). Here, we present an atomic-scale defect engineering strategy to improve the thermoelectric properties of graphene using embedded high-angle tilt boundary (HATB) domains in graphene films. These HATB domains serve as both energy filtering sites to filter out lower-energy charge carriers and scattering sites for phonons. Compared to the conventionally grown chemical vapor deposited graphene, the graphene with HATB domains shows an improved Seebeck coefficient (50.1 vs 21.1 μV K-1) and reduced thermal conductivity (382 vs 952 W m-1K-1), resulting in a ZT value that is ∼7 times greater at 350 K. This defect engineering strategy is promising not only for graphene-based materials but also for 2D materials, in general, where further research and optimization could overcome the limitations of conventional bulk thermoelectric materials in energy-harvesting systems.