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

Li, Qikai; Yu, Mao; Pang, Chunlin; Wu, Xinya; Wang, Shuaihua; Li, Huan; Wang, Yupeng; Liu, Weishu et al. · Nat Commun · 2025

basic_science · Level V

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Abstract

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<sub>CR</sub>) 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 KI<sub>3</sub>/KI and K<sub>3</sub>Fe(CN)<sub>6</sub>/K<sub>4</sub>Fe(CN)<sub>6</sub> redox couples, both utilizing the same counter-ion K<sup>+</sup> for regeneration, the t-ITC device attains a peak energy density of 3.28 kJ m<sup>-2</sup> 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.