Efficient Debundling of Few-Walled Carbon Nanotubes by Wrapping with Donor–Acceptor Polymers for Improving Thermoelectric Properties

Organic thermoelectric (TE) materials have great potential as sustainable energy sources for powering flexible and wearable electronic devices via harvesting of human body heat. Recent advances in soluble conjugated polymer/carbon nanotube (CNT) composites have facilitated achievement of high TE power factors. However, the effects of conjugated polymers on the debundling and electrical percolation of CNTs and on the TE properties of their composites are not yet fully understood. Herein, we introduce a novel type of polymer/CNT composite composed of a donor–acceptor (D–A)-type polymer and few-walled CNTs (FWCNTs). Three kinds of D–A polymers are employed to disperse FWCNTs, and the photophysical, morphological, and TE properties of the resulting polymer/FWCNT composites are compared with those of composites composed of FWCNTs dispersed with conventional donor-only poly(3-hexylthiophene). The results reveal that the strong intermolecular interaction forces and high backbone planarity of the D–A polymers facilitate effective debundling of FWCNTs, which results in much smaller bundle sizes. Consequently, the D–A polymer/FWCNT composite films show superior electrical percolation and TE performances with improved power factors of up to 459 μW/mK2. Finally, we demonstrate the feasibility of the D–A polymer/FWCNT composites for use in the fabrication of a flexible TE generator, which shows a maximum power output of 210 nW at a temperature gradient of 20 K.