Abstract

Single-walled carbon nanotubes (SWCNTs) have the potential for application in thermoelectric energy generators owing to their advantages, such as good charge-carrier transport properties, mechanical flexibility and robustness, and tunability of polarity. However, the fabrication of SWCNTs still remains a problem due to its complexity and high cost. In this paper, we propose an approach for the direct formation of free-standing SWCNT films from as-grown SWCNT mats without any dispersion or separation processes. We used this approach to develop high-performance SWCNT-based thermoelectric leg materials. The as-grown SWCNT mats were synthesized by an enhanced direct injection pyrolytic synthesis (eDIPS) method. The selectivity of the tube diameter for the eDIPS method clarified the dependence of the thermoelectric performance of the free-standing SWCNT films on the tube diameter. The Seebeck coefficients and thermal conductivities were found to correlate with the tube diameter and agreed with the theoretical predictions. Owing to the dispersion-free film formation, our SWCNT films afforded large thermoelectric power factors. In particular, a power factor of 350 μW/(m K2) was obtained for the mean tube diameter of 1.7 nm without any semiconductor extraction or doping treatments. Our approach allowed the fabrication of thermoelectric legs with an arbitrary size; thus, it offers a useful strategy for the simpler, cheaper, and low-waste manufacturing of high-performance organic thermoelectric devices.

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