Thermally chargeable supercapacitors (TCSC) have emerged as promising ionic thermoelectric devices for harvesting low-grade waste heat, but their practical implementation is limited by insufficient mechanical robustness, humidity sensitivity, and Seeb...
Thermally chargeable supercapacitors (TCSC) have emerged as promising ionic thermoelectric devices for harvesting low-grade waste heat, but their practical implementation is limited by insufficient mechanical robustness, humidity sensitivity, and Seebeck coefficient. In this study, a thermally chargeable hybrid supercapacitor (TCSC) was developed using a NiMn-LDH and PSSH/SOR/PVA electrolyte designed for high ionic mobility and environmental stability. The NiMn-LDH electrode provided a large active area through its layered double hydroxide structures (LDHs), enabling combining Soret and thermogalvanic effect. The electrolyte exhibited self-healing property, ionic conductivity of 6.09 mS/cm, thermal conductivity of 0.46 W/m∙K, elongation at break of ~350%, and water retention ratio (>90%) derived from the hydrogen bond network formed by D-sorbitol. These properties ensured stable ion diffusion and sustained temperature gradients during operation. Under a 10 – 20 K temperature gradient, the NiMn-LDH//carbon system achieved a Seebeck coefficient of 2.06 mV/K, a 21.18% enhancement over the NF//NF system. Energy density reached 8,742 J/m2 after 24 h, exceeding the NF//NF system (301.5 J/m2). A practical demonstration using a series-connected TCHS with a 1.8 V supply successfully powered an LED, confirming supplementary voltage operation. Overall, this work establishes a flexible, humidity-stable, and all-solid state TCHS capable of efficient heat-to-electric energy conversion with potential for self-powered wearable electronics and IoT application in real environmental conditions.