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Thermoresponsive ether-based electrolyte for wide temperature operating lithium metal batteries

Rong Gu, Da Zhang, Shengtao Xu, Xiaoyu Guo, Yuan Xiao, Zhimeng Sheng, Qunjie Xu, Jinting Xu (), Sheng Zhu (), Kexuan Liao, Shuaiqi Gong, Penghui Shi () and YuLin Min ()
Additional contact information
Rong Gu: Shanghai University of Electric Power
Da Zhang: Tongji University
Shengtao Xu: Shanghai University of Electric Power
Xiaoyu Guo: Shanghai University of Electric Power
Yuan Xiao: Shanghai University of Electric Power
Zhimeng Sheng: Shanghai University of Electric Power
Qunjie Xu: Shanghai University of Electric Power
Jinting Xu: Shanghai University of Electric Power
Sheng Zhu: Shanghai University of Electric Power
Kexuan Liao: Shanghai University of Electric Power
Shuaiqi Gong: Shanghai University of Electric Power
Penghui Shi: Shanghai University of Electric Power
YuLin Min: Shanghai University of Electric Power

Nature Communications, 2025, vol. 16, issue 1, 1-14

Abstract: Abstract Safe electrolytes operable over a wide temperature range are essential for lithium metal batteries, offering high redox interfacial stability, fast ion transport kinetics, and inherent safety. However, conventional electrolytes rarely achieve these characteristics simultaneously, typically sacrificing one to improve another. In this work, an ether-based thermoresponsive electrolyte is developed, in which the Li+ solvation structure varies with temperature and facilitates the formation of a polycrystalline electrode/electrolyte interface, enabling the desired properties under conventional salt concentrations. The solvation sheath is reconfigured by 1,3,5-trioxane, which promotes anion dissociation and enhances charge-transfer kinetics. Additionally, 1,3,5-trioxane triggers a cationic ring-opening polymerization of tetrahydrofuran at 60 °C, yielding oxidation-resistant ether-based polymers that improve high-temperature stability and safety. As a result, Li||LiNi0.8Co0.1Mn0.1O2 cells utilizing this electrolyte operate reliably across a broad temperature window (−60 to 60 °C). Furthermore, a practical 1.5 Ah Li|| Ni0.8Co0.1Mn0.1O2 pouch cell delivers a capacity retention of 74.7% after 60 cycles at −40 °C and 0.05 C (20 h charge/discharge), with a specific energy of 317.1 Wh kg−1(including packaging foil).

Date: 2025
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DOI: 10.1038/s41467-025-60524-8

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