Entropy-Driven Modulation of Ion Clustering and Polymer Crystallinity for Low-Temperature Lithium Metal Batteries.

IF 16.9 1区 化学 Q1 CHEMISTRY, MULTIDISCIPLINARY
Junze Guo,Weifeng Zou,Yaoxian Song,Xuyin Zhu,Haodong Zhou,Weidong Zhang,Fanghao Zhou,Tiefeng Li
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Abstract

Solid-state Li metal batteries have garnered significant attention for their intrinsic safety and high energy density. Among various solid-state electrolytes, solid polymer electrolytes (SPEs) offer their excellent processability and interfacial compatibility but suffer from the formation of large ionic clusters and crystallization, which hinder Li+ transport and desolvation, particularly at low temperatures (e.g., deep-sea conditions). In this study, a multicomponent strategy is adopted to enhance the configurational entropy of SPEs, resulting in a 2-fold reduction in Li cluster size and suppression of polymer crystallization. These changes facilitate rapid desolvation and promote the formation of a high-entropy solid electrolyte interphase. Owing to these benefits, the resulting SPEs exhibit an 8.5-fold improvement in ionic conductivity at -20 °C (0.17 mS cm-1). The Li/Cu cells exhibit an impressive average Coulombic efficiency (CE) of 98.59% over 300 cycles at room temperature, and maintain nearly unchanged CE even after a temperature drop to -20 °C. Furthermore, the Li/LiFePO4 cells (N/P = 4) achieve a 13-fold capacity improvement and an average capacity retention of 91.49% after 500 cycles at -20°C (over 248 days). This strategy builds a new approach for high performance SPEs for practical low-temperature operation.
低温锂金属电池中离子聚类和聚合物结晶度的熵驱动调制。
固态锂金属电池以其固有的安全性和高能量密度而备受关注。在各种固态电解质中,固体聚合物电解质(spe)具有优异的可加工性和界面相容性,但存在较大离子团簇的形成和结晶问题,这阻碍了Li+的传输和溶解,特别是在低温(例如深海条件)下。在本研究中,采用多组分策略来增强spe的构型熵,从而使Li簇尺寸减小2倍,并抑制聚合物结晶。这些变化有利于快速脱溶,促进高熵固体电解质界面相的形成。由于这些优点,所得的spe在-20°C (0.17 mS cm-1)时的离子电导率提高了8.5倍。在室温下,锂/铜电池在300次循环中显示出令人印象深刻的平均库仑效率(CE)为98.59%,即使在温度降至-20°C后也几乎保持不变。此外,锂/LiFePO4电池(N/P = 4)在-20°C下循环500次(超过248天)后,容量提高了13倍,平均容量保持率为91.49%。该策略为实际低温运行的高性能spe构建了一种新的方法。
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来源期刊
CiteScore
26.60
自引率
6.60%
发文量
3549
审稿时长
1.5 months
期刊介绍: Angewandte Chemie, a journal of the German Chemical Society (GDCh), maintains a leading position among scholarly journals in general chemistry with an impressive Impact Factor of 16.6 (2022 Journal Citation Reports, Clarivate, 2023). Published weekly in a reader-friendly format, it features new articles almost every day. Established in 1887, Angewandte Chemie is a prominent chemistry journal, offering a dynamic blend of Review-type articles, Highlights, Communications, and Research Articles on a weekly basis, making it unique in the field.
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