Thermoelectric technology that utilizes thermodynamic effects to convert thermal energy into electrical energy has greatly expanded wearable health monitoring, personalized detecting, and communicating applications. Encouragingly, thermoelectric technology assisted by artificial intelligence exerts great development potential in wearable electronic devices that rely on the self-sustainable operation of human body heat. Ionic thermoelectric (i-TE) devices that possess high Seebeck coefficients and a constant and stable electrical output are expected to achieve an effective conversation of thermal energy harvesting. Herein, we developed an i-TE paster for thermal chargeable energy storage, temperature-triggered material recognition, contact/non-contact temperature detection, and photo thermoelectric conversion applications. An all-solid-state organic ionic gel electrolyte (PVDF-HFP-PEO gel) with onion epidermal cells-like structure was sandwiched between two electrodes, which take full advantage of a synergy between the Soret effect and the polymer thermal expansion effect, thus achieving the enhanced ZT value up to 900% compared with the PEO-free electrolyte. The i-TE device delivers a Seebeck coefficient of 28 mV K−1, a maximum energy conversion efficiency of 1.3% in performance, and ultra-thin and skin-attachable properties in wearability, which demonstrate the great potential and application prospect of the i-TE paster in self-sustainable wearable electronics.
