Promoting the feasibility of thermoelectric (TE) devices toward wearable power generator application has sparked extensive interest for next-generation electronics. However, the lack of air-stable and high-performance n-type TE materials, which lag far behind those of p-type TE materials, and the deficiency of reasonable device structure design have always restricted the development of wearable thermoelectrics. Herein, we prepare a high-performance and air-stable n-type carbon nanotube fiber (CNTF) by multistep treatment and design a three-dimensional (3D) wavy-structured TE device to address the mentioned challenges. The multistep treatment including oleylamine (OA) doping followed by annealing process (250 °C) can contribute to an enhanced Seebeck coefficient of ~ −80 μV K⁻¹ and an increased power factor of ~545 μW m⁻¹ K⁻². Notably, it is found that the n-type CNTF prepared by this multistep treatment shows good air stability, which effectively diminishes the malignant effects of conventional annealing process on the air stability. Based on the optimized TE performance of an alternately p/n doped CNTF, the prepared wavy-structured generator integrated with two p-n couples can sustainably yield a stable amplitude of ~1.3 mV in voltage response during multiple fingering cycles and output a maximum power of ~8 nW under a temperature difference of ~5.7 K when the top of the device comes into contact with fingers. This paper provides a new insight into developing high-performance/air-stable n-type carbon nanotubes (CNTs) materials and designing reasonable device structure toward wearable applications.

促进热电(TE) 设备在可穿戴发电机应用中的可行性已经激发了对下一代电子产品的广泛兴趣。然而，空气稳定、高性能的n型热电材料的缺乏远远落后于p型热电材料，以及器件结构设计合理的不足一直制约着可穿戴热电材料的发展。在此，我们通过多步处理制备了高性能且空气稳定的 n 型碳纳米管纤维 (CNTF)，并设计了三维 (3D) 波浪结构的 TE 器件以解决上述挑战。包括油胺 (OA) 掺杂和退火工艺 (250 °C) 在内的多步处理有助于提高约 -80 μV K ^{-1 的}塞贝克系数功率因数增加~545 μW m ^-1  K ^-2. 值得注意的是，通过这种多步处理制备的n型CNTF表现出良好的空气稳定性，有效地减少了常规退火工艺对空气稳定性的不利影响。基于交替 p/n 掺杂 CNTF 的优化 TE 性能，制备的集成有两个 pn 对的波浪结构发生器可以在多个指法循环期间持续产生 ~1.3 mV 的稳定幅度电压响应，并输出 ~当设备顶部与手指接触时，在约 5.7 K 的温差下为 8 nW。本文为开发高性能/空气稳定的 n 型碳纳米管 (CNT) 材料和为可穿戴应用设计合理的设备结构提供了新的见解。