Ultrastrong and Reusable Solar‒Thermal‒Electric Generators by Economical Starch Vitrimers

In frigid regions, it is imperative to possess functionality materials that are ultrastrong, reusable, and economical, providing self-generated heat and electricity. One promising solution is a solar‒thermal‒electric (STE) generator, composed of solar‒thermal conversion phase change composites (PCCs) and temperature-difference power-generation-sheets. However, the existing PCCs face challenges with conflicting requirements for solar‒thermal conversion efficiency and mechanical robustness, mainly due to monotonous functionalized aerogel framework. Herein, a novel starch vitrimer aerogel is proposed that incorporates orientational distributed carboxylated carbon nanotubes (CCNT) to create PCC. This innovative design integrates large through-holes, mechanical robustness, and superior solar‒thermal conversion. Remarkably, PCC with only 0.8 wt.% CCNT loading achieves 85.8 MPa compressive strength, 102.4 °C at 200 mW cm^-2 irradiation with an impressive 92.9% solar-thermal conversion efficiency. Noteworthy, the STE generator assembled with PCC harvests 99.1 W m^-2 output power density, surpassing other reported STE generators. Strikingly, even under harsh conditions of -10 °C and 10 mW cm^‒2 irradiation, the STE generator maintains 20 °C for PCC with 325 mV output voltage and 45 mA current, showcasing enhanced electricity generation in colder environments. This study introduces a groundbreaking STE generator, paving the way for self-sufficient heat and electricity supply in cold regions.