Long‐Term Serviceable Ionic Thermoelectric Hydrogel with Temperature and Moisture Dual‐Driven Waste Energy Harvesting Capability

Despite the substantial progress in developing high-performance quasi-solid hydrogels based on ionic thermophoretic migration, ionic thermoelectric materials (i-TEs) show unsatisfactory long-lasting stability caused by ionic migration failures and de-electrolytes. In this work, by enriching oxygen-containing functional groups in the gel network and constructing oriented ionic transport nanochannels, an innovative approach is presented to reach long-term service and reusability for i-TEs without sacrificing their TE properties. The as-prepared hydrogel with thermopower of 17.0 ± 1.0 mV K^-1 stables at 82% of its original performance when immersed in the electrolyte. Notably, even after being air-dried for 135 days, its thermopower returns to 87% of the original value through replenishing electrolyte solution and its 3D shape fully recovers. Meanwhile, the dual-driven nature for moisture and temperature as well as the pH sensitivity of this network is systematically investigated. The maximum output voltage of a single sample reaches 0.215 V at a ΔT of 3.7 K, and it works continuously for more than 26 h. This study offers a new approach to overcoming the short-term service bottleneck of i-TEs and provides a practical scheme for the multi-source drive of self-powered TE equipment.