Tailoring tetrahedral and pair-correlation entropies of glass-forming liquids for energy storage applications at ultralow temperatures

Meijia Qiu, Peng Sun, Yuxuan Liang, Jian Chen, Zhong Lin Wang () and Wenjie Mai ()
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Meijia Qiu: Jinan University
Peng Sun: Jinan University
Yuxuan Liang: Jinan University
Jian Chen: Sun Yat-Sen University
Zhong Lin Wang: Chinese Academy of Sciences
Wenjie Mai: Jinan University

Nature Communications, 2024, vol. 15, issue 1, 1-10

Abstract: Abstract Aqueous solution experiences either crystallization or vitrification as being cooled, yet the mechanism of this bifurcation is confused. Since the glass-transition temperature Tg is much lower than the melting temperature, we herein propose an entropy-driven glass-forming liquid (EDGFL) as an attractive concept to develop anti-freezing electrolytes. The Tg is delicately modulated via regulating local structural orders to avoid the energy-driven ice crystallization and enter an entropy-driven glass transition, which can be theoretically explained by the competitive effect between tetrahedral entropy of water and pair correlation entropy related to ions. The constructive EDGFL with a low Tg of −128 °C and a high boiling point of +145 °C enables stable energy storage over an ultra-wide temperature range of −95~+120 °C, realizes superior AC linear filtering function at −95 °C, and helps improve the performance of aqueous Zn-ion batteries at ultralow temperatures. This special electrolyte will provide both theoretical and practical directions for developing anti-freezing energy storage systems adapting to frigid environment.

Date: 2024
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DOI: 10.1038/s41467-024-54449-x

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