Regulating the Solvation Structure in Polymer Electrolytes for High-Voltage Lithium Metal Batteries

Yuncong Liu, Zhekai Jin, Zeyu Liu, Hao Xu, Furong Sun, Xue Qiang Zhang, Tao Chen*, Chao Wang*

*此作品的通讯作者

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摘要

Solid polymer electrolytes are promising electrolytes for safe and high-energy-density lithium metal batteries. However, traditional ether-based polymer electrolytes are limited by their low lithium-ion conductivity and narrow electrochemical window because of the well-defined and intimated Li+-oxygen binding topologies in the solvation structure. Herein, we proposed a new strategy to reduce the Li+-polymer interaction and strengthen the anion-polymer interaction by combining strong Li+-O (ether) interactions, weak Li+-O (ester) interactions with steric hindrance in polymer electrolytes. In this way, a polymer electrolyte with a high lithium ion transference number (0.80) and anion-rich solvation structure is obtained. This polymer electrolyte possesses a wide electrochemical window (5.5 V versus Li/Li+) and compatibility with both Li metal anode and high-voltage NCM cathode. Li||LiNi0.5Co0.2Mn0.3O2 full cells with middle-high active material areal loading (~7.5 mg cm−2) can stably cycle at 4.5 V. This work provides new insight into the design of polymer electrolytes for high-energy-density lithium metal batteries through the regulation of ion-dipole interactions.

源语言英语
文章编号e202405802
期刊Angewandte Chemie - International Edition
63
34
DOI
出版状态已出版 - 19 8月 2024

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Liu, Y., Jin, Z., Liu, Z., Xu, H., Sun, F., Zhang, X. Q., Chen, T., & Wang, C. (2024). Regulating the Solvation Structure in Polymer Electrolytes for High-Voltage Lithium Metal Batteries. Angewandte Chemie - International Edition, 63(34), 文章 e202405802. https://doi.org/10.1002/anie.202405802