Abstract

In this study, two conjugated polymers (CPs) featuring poly(phenylene butadiynylene) (PPB) were meticulously synthesized and composited with single-walled carbon nanotubes (SWCNTs) to investigate their thermoelectric properties and fabricate wearable thermoelectric generators (TEGs). These CPs, designated as P1 and P2, were tailored with distinct side chain configurations by incorporating 2-butyloctyloxy and 6-(methyldioctylsilyl)hexyloxy groups, respectively. Notably, P2, characterized by longer side chains with branchpoints farther from the backbone, exhibited planar backbone structure and enhanced solubility, consequently engendering stronger π–π interaction with SWCNTs and facilitating the disperse of SWCNTs through polymer wrapping at bundle surface. Such characteristics therefore contributed to the superior thermoelectric performances of the P2/SWCNTs nanocomposite, yielding a higher power factor (PF) of 216.5 μW m−1 K−2 for the spin-coated film. Furthermore, the corresponding wearable TEGs, which were constructed through spray-coating with 14 legs, resulted in an output power of approximately 49.6 nW under a temperature difference of 25 K, exhibiting successful harvesting of waste heat. Further applications also demonstrated operational efficacy under diverse conditions. These findings not only underscored the significance of side chain engineering in tailoring the thermoelectric properties of CP/SWCNTs nanocomposites but also demonstrated the feasibility of fabricating high-performance wearable thermoelectric devices applicable in versatile contexts.

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