Tailoring water structure with high-tetrahedral-entropy for antifreezing electrolytes and energy storage at −80 °C

Meijia Qiu, Peng Sun, Kai Han, Zhenjiang Pang, Jun Du, Jinliang Li, Jian Chen, Zhong Lin Wang () and Wenjie Mai ()
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Meijia Qiu: Guangdong Provincial Engineering Technology Research Center of Vacuum Coating Technologies and New Energy Materials, Department of Physics, Jinan University
Peng Sun: Guangdong Provincial Engineering Technology Research Center of Vacuum Coating Technologies and New Energy Materials, Department of Physics, Jinan University
Kai Han: Guangdong Provincial Engineering Technology Research Center of Vacuum Coating Technologies and New Energy Materials, Department of Physics, Jinan University
Zhenjiang Pang: Beijing Smart-Chip Microelectronics Technology Co., Ltd
Jun Du: Beijing Smart-Chip Microelectronics Technology Co., Ltd
Jinliang Li: Guangdong Provincial Engineering Technology Research Center of Vacuum Coating Technologies and New Energy Materials, Department of Physics, Jinan University
Jian Chen: Instrumental Analysis and Research Center, Sun Yat-Sen University
Zhong Lin Wang: Beijing Institute of Nanoenergy and Nanosystems, Chinese Academy of Sciences
Wenjie Mai: Guangdong Provincial Engineering Technology Research Center of Vacuum Coating Technologies and New Energy Materials, Department of Physics, Jinan University

Nature Communications, 2023, vol. 14, issue 1, 1-10

Abstract: Abstract One of unsolved puzzles about water lies in how ion-water interplay affects its freezing point. Here, we report the direct link between tetrahedral entropy and the freezing behavior of water in Zn2+-based electrolytes by analyzing experimental spectra and molecular simulation results. A higher tetrahedral entropy leads to lower freezing point, and the freezing temperature is directly related to the entropy value. By tailoring the entropy of water using different anions, we develop an ultralow temperature aqueous polyaniline| |Zn battery that exhibits a high capacity (74.17 mAh g−1) at 1 A g−1 and −80 °C with ~85% capacity retention after 1200 cycles due to the high electrolyte ionic conductivity (1.12 mS cm−1). Moreover, an improved cycling life is achieved with ~100% capacity retention after 5000 cycles at −70 °C. The fabricated battery delivers appreciably enhanced performance in terms of frost resistance and stability. This work serves to provide guidance for the design of ultralow temperature aqueous batteries by precisely tuning the water structure within electrolytes.

Date: 2023
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DOI: 10.1038/s41467-023-36198-5

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