Synergy between gelatin hydrogels and electrodes for adjustable and thermally stable ionic thermoelectric supercapacitors

Gelatin-based ionic hydrogels are flexible, bio-compatible, and abundant materials, showing immense potential as quasi-solid-state electrolytes in energy conversion and storage applications. Recent studies highlighted the critical synergy between hydrogel electrolytes and electrodes on the thermopower and energy density in emerging ionic thermoelectric (i-TE) devices. In this work, the significant impact from electrodes to the thermoelectric response of gelatin hydrogels is explored and explained at the molecular level. A universal negative offset in the thermopower is observed when substituting the conventional Cu foil by carbon-based paper (CBP) electrodes. This is attributed to the electrolyte infiltration and strong cation restriction on the CBP electrodes, which facilitates anion thermodiffusion. The thermopowers of Gelatin-CsCl change from p- (0.1–0.5 mV K−1) to n-type (up to −2.89 ± 0.34 mV K−1) and remain thermally stable at a large temperature difference of −36.8 K. The power factor and average power density in the ionic thermoelectric supercapacitors (ITESCs) made from Gelatin-0.02 M CsCl and CBP electrodes reach 2.13 ± 0.50 μW m−1 K−2 and 145.37 μW m−2 at a small temperature difference of −7.7 K. Furthermore, the highest normalized instantaneous power density achieved during the quasi-continuous charge–discharge cycles is 39.42 μW m−2 K−2, among the best ITESCs. This work provides fundamental insights into the previously overlooked synergy between gelatin hydrogels and electrodes for adjustable and thermally stable i-TE conversion and energy storage devices.