Low-grade heat (below 373 K) is abundant and ubiquitous, but mostly wasted due to the lack of cost-effective recovery technologies. The liquid-state thermocell (LTC), an inexpensive and scalable thermoelectric device, may be commercially viable for harvesting low-grade heat energy if its Carnot-relative efficiency (ηr) reaches ~5%, which is a challenging metric to achieve experimentally. We used a thermosensitive crystallization and dissolution process to induce persistent concentration gradient of redox ions, a highly enhanced Seebeck coefficient (~3.73 mV K–1), and suppressed thermal conductivity in LTCs. As a result, we achieved a high ηr of 11% for LTCs near room temperature, and a substantially decreased cost-performance of our LTC. Our device demonstration offers promise for cost-effective low-grade heat harvesting.

Thermogalvanic cells offer a cheap, flexible and scalable route for directly converting heat into electricity. However, achieving a high output voltage and power performance simultaneously from low-grade thermal energy remains challenging. Here, we introduce strong chaotropic cations (guanidinium) and highly soluble amide derivatives (urea) into aqueous ferri/ferrocyanide ([Fe(CN)6]4−/[Fe(CN)6]3−) electrolytes to significantly boost their thermopowers. The corresponding Seebeck coefficient and temperature-insensitive power density simultaneously increase from 1.4 to 4.2 mV K−1 and from 0.4 to 1.1 mW K−2 m−2, respectively. The results reveal that guanidinium and urea synergistically enlarge the entropy difference of the redox couple and significantly increase the Seebeck effect. As a demonstration, we design a prototype module that generates a high open-circuit voltage of 3.4 V at a small temperature difference of 18 K. This thermogalvanic cell system, which features high Seebeck coefficient and low cost, holds promise for the efficient harvest of low-grade thermal energy.

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