Multifunctional electrolyte additive for high power lithium metal batteries at ultra-low temperatures

Weili Zhang (), Yang Lu, Qingqing Feng, Hao Wang, Guangyu Cheng, Hao Liu, Qingbin Cao, Zhenjun Luo, Pan Zhou, Yingchun Xia, Wenhui Hou, Kun Zhao, Chunyi Du and Kai Liu ()
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Weili Zhang: Tsinghua University
Yang Lu: Tsinghua University
Qingqing Feng: Tsinghua University Hefei Institute for Public Safety Research
Hao Wang: Tsinghua University Hefei Institute for Public Safety Research
Guangyu Cheng: Shanghai Institute of Space Power-Sources
Hao Liu: Tsinghua University Hefei Institute for Public Safety Research
Qingbin Cao: Xinyuan Qingcai Technology Co., Ltd
Zhenjun Luo: Tsinghua University Hefei Institute for Public Safety Research
Pan Zhou: Tsinghua University
Yingchun Xia: Tsinghua University
Wenhui Hou: Tsinghua University
Kun Zhao: Tsinghua University Hefei Institute for Public Safety Research
Chunyi Du: Tsinghua University Hefei Institute for Public Safety Research
Kai Liu: Tsinghua University

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

Abstract: Abstract Ultra-low-temperature lithium metal batteries face significant challenges, including sluggish ion transport and uncontrolled lithium dendrite formation, particularly at high power. An ideal electrolyte requires high carrier ion concentration, low viscosity, rapid de-solvation, and stable interfaces, but balancing these attributes remains a formidable task. Here, we design and synthesize a multifunctional additive, perfluoroalkylsulfonyl quaternary ammonium nitrate (PQA-NO3), which features both cationic (PQA+) and anionic (NO3−) components. PQA+ reacts in situ with lithium metal to form an inorganic-rich solid-electrolyte interphase (SEI) that enhances Li+ transport through the SEI film. NO3− creates an anion-rich, solvent-poor solvation structure, improving oxidation stability at the positive electrode/electrolyte interface and reducing Li+-solvent interactions. This allows ether-based electrolytes to achieve high voltage tolerance, increased ionic conductivity, and lower de-solvation energy barriers. The Li (40 µm)||NMC811 (3 mAh cm−2) coin cells with the developed electrolyte exhibited stable cycling at -60 °C and a 450 Wh kg−1 pouch cell retained 48.1% capacity at -85 °C, achieving a specific energy (except tabs and packing foil, same hereafter) of 171.8 Wh kg−1. Additionally, the pouch cell demonstrated a discharge rate of 3.0 C at -50 °C, reaching a specific power (except tabs and packing foil, same hereafter) of 938.5 W kg−1, indicating the electrolyte’s suitability for high-rate lithium metal batteries in extreme low-temperature environments.

Date: 2025
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DOI: 10.1038/s41467-025-58627-3

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