Tailoring polymer electrolyte solvation for 600 Wh kg−1 lithium batteries

Xue-Yan Huang, Chen-Zi Zhao (), Wei-Jin Kong, Nan Yao, Zong-Yao Shuang, Pan Xu, Shuo Sun, Yang Lu, Wen-Ze Huang, Jin-Liang Li, Liang Shen, Xiang Chen, Jia-Qi Huang, Lynden A. Archer and Qiang Zhang ()
Additional contact information
Xue-Yan Huang: Tsinghua University
Chen-Zi Zhao: Tsinghua University
Wei-Jin Kong: Tsinghua University
Nan Yao: Tsinghua University
Zong-Yao Shuang: Tsinghua University
Pan Xu: Tsinghua University
Shuo Sun: Tsinghua University
Yang Lu: Tsinghua University
Wen-Ze Huang: Tsinghua University
Jin-Liang Li: Tsinghua University
Liang Shen: Tsinghua University
Xiang Chen: Tsinghua University
Jia-Qi Huang: Beijing Institute of Technology
Lynden A. Archer: Cornell University
Qiang Zhang: Tsinghua University

Nature, 2025, vol. 646, issue 8084, 343-350

Abstract: Abstract Polymer electrolytes paired with lithium-rich manganese-based layered oxide (LRMO) cathodes and anode-free cell design are considered one of the most promising high-energy-density and high-safety systems1–4. However, the unstable anode morphological changes and the irreversible anionic reactions at the electrolyte–cathode interfaces induce oxygen escape and catalytic decomposition of polymer electrolytes, resulting in severe interfacial degradation and poor cycling stability. Here we design an in-built fluoropolyether-based polymer electrolyte composed of strongly solvating polyether and weakly solvating fluorohydrocarbon pendants, creating an anion-rich solvation structure and thus anion-derived fluorine-rich interfacial layers on the cathode and anode to resist interfacial issues. The LRMO cathode exhibits improved oxygen redox reversibility with substantially reduced oxygen-involving interfacial side reactions. This quasi-solid-state polymer electrolyte with 30 wt% trimethyl phosphate enables an LRMO cathode with a reversible high-areal-capacity cycling (>8 mAh cm−2) in pouch cells and long-term stability (>500 cycles at 25 °C) in coin cells, respectively. The pouch cells exhibit an energy density of 604 Wh kg−1 (1,027 Wh l−1) and excellent safety under a nail penetration at a fully charged condition. Our work, therefore, provides a promising direction for creating practical high-energy-density and high-safety lithium batteries.

Date: 2025
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DOI: 10.1038/s41586-025-09565-z

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