Temperature adaptive self-regenerating ionic thermoelectric cycles for time domain thermal energy harvesting

The rising demand for sustainable energy solutions has promoted significant interest in ionic thermoelectric materials, which convert low-grade waste heat into electrical energy through spatial temperature gradients. However, diurnal temperature variations, which offer potential for location-independent time-domain thermal energy, remain largely unexplored. To overcome the challenges of harvesting spatially limited thermal energy, this study presents an ionic thermoelectric cycle (t-ITC) designed for time-domain thermal energy harvesting, incorporating two gels with contrasting temperature coefficients. A temperature-adaptive self-regeneration (TASR) strategy is proposed to set the critical regeneration temperature (T_CR) at the midpoint of temperature fluctuations, facilitating long-term device operation. The regeneration criteria are defined as neutralization of the electrochemical potential difference between separated cells, and a method based on shared counter-ion self-balancing is introduced. Employing a polyacrylamide-polyvinylpyrrolidone (PAM-PVP) matrix with KI₃/KI and K₃Fe(CN)₆/K₄Fe(CN)₆ redox couples, both utilizing the same counter-ion K⁺ for regeneration, the t-ITC device attains a peak energy density of 3.28 kJ m^–2 per cycle and a relative Carnot efficiency of 8.39% with 70% heat recuperation, under cycling conditions between 60 °C and 10 °C. This work highlights the potential of t-ITC devices for global-scale time-domain thermal energy on a global scale, across diverse environments, such as hot deserts and cold plateaus. © The Author(s) 2025.