Self-Supporting PAM/PEDOT:PSS Thermoelectric Devices Enhanced by Metasurface Radiative Cooling

The rapid development of wearable electronics has created a demand for flexible, lightweight, and sustainable power-supply technologies. The persistent temperature difference between the human body and the environment provides a low-grade thermal source for thermoelectric energy harvesting. However, traditional flexible thermoelectric devices still face limited self-supporting capabilities and difficulties in maintaining sufficiently low cold-side temperatures. Here, we designed a passively radiative-cooled thermoelectric film (PRT film) by integrating a PAM/PEDOT:PSS self-supporting thermoelectric composite layer with a polymer metamaterial radiative cooling (PMRC) film. The PAM/PEDOT:PSS layer serves as a self-supporting thermoelectric conversion component for harvesting low-grade heat, while the PMRC film layer acts as a passive cold-side regulator without energy input to lower the cold-side temperature and enhance the temperature gradient. By optimizing the PAM content, the PAM/PEDOT:PSS composite material with 85 wt% PAM achieved the highest power factor of 72.3 μW m−1 K−2. Under a temperature difference of 39 °C, the optimized PAM/PEDOT:PSS sample provided an open-circuit voltage of 0.47 V, a maximum output power of 1.1 μW, and a power density of 11.2 μW cm−2. According to the temperature-difference enhancement measured in experiments and the independently obtained load characteristics, the integration of PMRC films is expected to increase the maximum output power from 1.1 to 1.4 μW, with the corresponding power density rising from 11.2 to 14.25 μW cm−2, representing a 27.2% enhancement. This work demonstrates the feasibility of passive radiative cold-side regulation in enhancing low-level thermoelectric energy harvesting for wearable applications.