The Enhanced Thermoelectric and Mechanical Performance of Polythiophene/Single-Walled Carbon Nanotube Composites with Polar Ethylene Glycol Branched-Chain Modifications

In order to develop flexible thermoelectric materials with thermoelectric and mechanical properties, in this study, we designed and synthesized polythiophene derivatives with branched ethylene glycol polar side-chains named P3MBTEMT, which were used in combination with single-walled carbon nanotubes (SWCNTs) to prepare composite thin films and flexible thermoelectric devices. A comparison was made with a polymer named P3(TEG)T, which has a polar alkoxy linear chain. The UV-vis results indicated that the larger steric hindrances of the branched ethylene glycol side-chain in P3MBTEMT could inhibit its self-aggregation and had a stronger interaction with the SWCNTs compared to that of P3(TEG)T, which was also confirmed using Raman spectroscopy. When the mass ratio of SWCNTs to P3MBTEMT was 9:1 (represented as P3MBTEMT/SWCNTs-0.9), the composite film exhibited the highest thermoelectric properties with a power factor of 446.98 μW m−1 K−2, which was more than two times higher than that of P3(TEG)T/SWCNTs-0.9 (215.08 μW m−1 K−2). The output power of the thermoelectric device with P3MBTEMT/SWCNTs-0.9 was 2483.92 nW at 50 K, which was 1.66 times higher than that of P3(TEG)T/SWCNTs-0.9 (1492.65 nW). Furthermore, the P3MBTEMT/SWCNTs-0.5 showed superior mechanical properties compared to P3(TEG)T/SWCNTs-0.5. These results indicated that the mechanical and thermoelectric performances of polymer/SWCNT composites could be significantly improved by adding polar branched side-chains to conjugated polymers. This study provided a new strategy for creating high-performing novel flexible thermoelectric materials.