Thermoelectric generators (TEGs) based on thermogalvanic cells can convert low-temperature waste heat into electricity. Organic redox couples are well-suited for wearable devices due to their nontoxicity and the potential to enhance the ionic Seebeck coefficient through functional-group modifications. Pyrazine-based organic redox couples with different functional groups is comparatively analyzed through cyclic voltammetry under varying temperatures. The results reveal substantial differences in entropy changes with temperature and highlight 2,5-pyrazinedicarboxylic acid dihydrate (PDCA) as the optimal candidate. How the functional groups of the pyrazine compounds impact the ionic Seebeck coefficient is examined, by calculating the electrostatic potential based on density functional theory. To evaluate the thermoelectric properties, PDCA is integrated in different concentrations into a double-network hydrogel comprising poly(vinyl alcohol) and polyacrylamide. The resulting champion device exhibits an impressive ionic Seebeck coefficient (S) of 2.99 mV K, with ionic and thermal conductivities of ≈67.6 µS cm and ≈0.49 W m K, respectively. Finally, a TEG is constructed by connecting 36 pieces of 20 × 10 m PDCA-soaked hydrogel in series. It achieves a maximum power output of ≈0.28 µW under a temperature gradient of 28.3 °C and can power a small light-emitting diode. These findings highlight the significant potential of TEGs for wearable devices.
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