Flexible and air-stable n-type oleylamine/carbon nanotube hybrid yarns for high-performance wearable thermoelectric generators

[Display omitted] •A flexible n-type oleylamine/carbon nanotube hybrid yarn with a power factor of 876.25 μW m-1 K-2 was developed.•The oleylamine/carbon nanotube hybrid yarn exhibited a stable n-type behavior for over 370 days of continuous exposure to air.•The constructed thermoelectric generator yielded an output voltage of 705.94 mV and a maximum output power of 44.34 μW. Wearable thermoelectric generators (TEGs), envisioned to harness the temperature gradient (ΔT) between the human body and the environment into electricity, hold great promise for powering wearable electronics. However, their practical application has been hampered by the scarcity of flexible n-type thermoelectric (TE) materials boasting both high performance and long-term air stability. Here, we introduce a significant advancement by developing an n-type TE material through immersing carbon nanotube yarn (CNTY) into an oleylamine (OAm)/ethanol solution, followed by drying under atmospheric conditions. The resulting OAm/CNTY exhibits a Seebeck coefficient of -80.48 μV K-1, an electrical conductivity of 1353.18 S cm-1 and a power factor of 876.25 μW m-1 K-2, all while exhibiting exceptional mechanical flexibility. Notably, this hybrid yarn maintains stable n-type behavior even after enduring exposure to air for over 370 days, surpassing previous n-type TE materials based on CNT fibers and CNTY. Leveraging this advancement, we construct a prototype wearable TEG by alternately embroidering pristine p-type CNTY and n-type OAm/CNTY into a polyester spacer fabric, electrically connecting them in series using conductive silver paint. The resulting wearable TEG, featuring with 150 p-n couples, yields an output voltage of 705.94 mV and a maximum output power of 44.34 μW at a ΔT of 40 K. This groundbreaking work opens new avenues for the development of high-performance, air-stable, and flexible n-type TE material, ushering in a new era for wearable TEGs.