Non-flammable and stable phosphate quasi-solid electrolyte with low salt concentration for lithium metal batteries

IF 9.6 1区材料科学 Q1 MATERIALS SCIENCE, MULTIDISCIPLINARY

Rare Metals Pub Date : 2025-02-28 DOI:10.1007/s12598-025-03239-5

Man-Ni Li, Fei Shen, Kai-Ming Wang, Zhe Zhang, Xiao-Gang Han

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Abstract

Lithium metal batteries face serious safety challenges caused by flammable organic electrolytes and the growth of lithium dendrite. Trimethyl phosphate (TMP) is a promising alternative for flammable carbonate electrolyte solvents owing to its nonflammable nature. But the low-concentration TMP-based electrolyte is unstable with the lithium metal anode. Here, a TMP-contained quasi-solid electrolyte (PIQSE) with porous polyimide (PI) as supporting skeleton is designed. The cross-linking structure generated by UV curing in PIQSE can lock the reactive TMP solvent to reduce its contact with Li metal. Besides, the PI supporting skeleton with high-temperature resistance can significantly enhance the thermal stability of PIQSE. The combination of PI and TMP prompts the high ionic conductivity and excellent nonflammability of PIQSE. The LiFePO₄/Li cell using PIQSE shows superior electrochemical performance in a wide temperature range from −10 to 60 °C. Furthermore, the cells with high-voltage cathode of LiNi_0.6Co_0.2Mn_0.2O₂ (NCM622) were matched with PIQSE exhibit good cyclic and rate performance. The NCM622/PIQSE/Li pouch cell was also fabricated. It exhibits a high discharge capacity of 182.9 mAh·g⁻¹, and can stably light up LEDs after folding and shearing tests, demonstrating broad prospects for highly safe energy storage applications.

Graphical abstract

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锂金属电池用不易燃、稳定、低盐浓度的磷酸盐类固体电解质

锂金属电池面临着易燃有机电解质和锂枝晶生长带来的严峻安全挑战。磷酸三甲酯（TMP）由于其不可燃性，是一种很有前途的可燃碳酸盐电解质溶剂替代品。但低浓度的tmp基电解液对锂金属阳极不稳定。本文设计了一种以多孔聚酰亚胺（PI）为支撑骨架的含tpmp准固体电解质（PIQSE）。PIQSE中紫外光固化产生的交联结构可以锁住活性TMP溶剂，减少其与Li金属的接触。此外，具有耐高温性能的PI支撑骨架可以显著提高PIQSE的热稳定性。PIQSE与TMP的结合使其具有高离子电导率和优异的不燃性。使用PIQSE的LiFePO4/Li电池在−10至60°C的宽温度范围内表现出优异的电化学性能。此外，与PIQSE匹配的高压阴极为LiNi0.6Co0.2Mn0.2O2 （NCM622）的电池具有良好的循环性能和速率性能。制备了NCM622/PIQSE/Li袋状电池。其放电容量高达182.9 mAh·g−1，且经过折叠和剪切测试后能够稳定点亮led，具有高度安全的储能应用前景。图形抽象

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来源期刊

Rare Metals 工程技术-材料科学：综合

CiteScore

12.10

自引率

12.50%

发文量

2919

审稿时长

2.7 months

期刊介绍： Rare Metals is a monthly peer-reviewed journal published by the Nonferrous Metals Society of China. It serves as a platform for engineers and scientists to communicate and disseminate original research articles in the field of rare metals. The journal focuses on a wide range of topics including metallurgy, processing, and determination of rare metals. Additionally, it showcases the application of rare metals in advanced materials such as superconductors, semiconductors, composites, and ceramics.