Constructing Quasi-Localized High-Concentration Solvation Structures to Stabilize Battery Interfaces in Nonflammable Phosphate-Based Electrolyte.

IF 14.3 1区 材料科学 Q1 CHEMISTRY, MULTIDISCIPLINARY
Chenyang Shi, Mengran Wang, Zari Tehrani, Bo Hong, Mengnan Wang, Rui Tan, Serena Margadonna, Yanqing Lai, Maria Magdalena Titirici
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Abstract

Flame-retardant phosphate-based electrolytes effectively enhance lithium-ion battery safety but suffer from poor compatibility with graphite anodes and high-voltage cathodes, hindering scalability. Fluorinated phosphates, though widely used, increase interfacial resistance at the anode, degrading performance. In this work, carbonate solvents with strong polarity are introduced to prevent tris(2,2,2-trifluoroethyl) phosphate (TFEP) from participating in the solvation structure of lithium ions. This strategy forms a quasi-localized high-concentration solvation structure, thereby restricting the reduction of TFEP and its impact on the graphite anode. The LiNi0.8Mn0.1Co0.1O2 (NCM811) | Graphite (Gr) pouch cell with optimized electrolyte exhibits a capacity retention rate of 80.1% after 370 cycles at 0.5C, which is much more stable than the electrolyte with TFEP-involved solvation structure (capacity retention rate: 47.1% after 300 cycles). The corresponding pouch cell with cut-off voltage to 4.5 V exhibits a capacity retention rate of 82.8% after 125 cycles, significantly outperforming cells employing commercial carbonate electrolytes (capacity retention rate: 56.9% after 125 cycles). Thus, the developed quasi-localized high-concentration solvation structure can effectively stabilize the electrode interface, greatly enhancing the cycling performance of phosphate-based flame-retardant electrolytes.

构建准局部高浓度溶解结构,稳定不易燃磷酸盐电解液中的电池界面
阻燃磷酸盐电解质可有效提高锂离子电池的安全性,但与石墨阳极和高压阴极的兼容性较差,阻碍了电池的可扩展性。氟化磷酸盐虽然应用广泛,但会增加阳极的界面电阻,降低性能。在这项工作中,引入了极性较强的碳酸盐溶剂,以防止磷酸三(2,2,2-三氟乙基)酯(TFEP)参与锂离子的溶解结构。这种策略形成了一种准局部高浓度溶解结构,从而限制了 TFEP 的还原及其对石墨负极的影响。采用优化电解质的 LiNi0.8Mn0.1Co0.1O2 (NCM811) | 石墨 (Gr) 袋式电池在 0.5C 温度下循环 370 次后,容量保持率达到 80.1%,比采用 TFEP 参与溶解结构的电解质(循环 300 次后容量保持率为 47.1%)稳定得多。截止电压为 4.5 V 的相应袋式电池在 125 次循环后的容量保持率为 82.8%,明显优于采用商业碳酸盐电解质的电池(125 次循环后的容量保持率为 56.9%)。因此,所开发的准局域高浓度溶解结构可有效稳定电极界面,大大提高磷酸盐基阻燃电解质的循环性能。
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来源期刊
Advanced Science
Advanced Science CHEMISTRY, MULTIDISCIPLINARYNANOSCIENCE &-NANOSCIENCE & NANOTECHNOLOGY
CiteScore
18.90
自引率
2.60%
发文量
1602
审稿时长
1.9 months
期刊介绍: Advanced Science is a prestigious open access journal that focuses on interdisciplinary research in materials science, physics, chemistry, medical and life sciences, and engineering. The journal aims to promote cutting-edge research by employing a rigorous and impartial review process. It is committed to presenting research articles with the highest quality production standards, ensuring maximum accessibility of top scientific findings. With its vibrant and innovative publication platform, Advanced Science seeks to revolutionize the dissemination and organization of scientific knowledge.
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