Liquid–liquid interfacial tension stabilized Li-metal batteries

Haijin Ji, Jingwei Xiang, Yong Li, Mengting Zheng, Lixia Yuan (), Yaqi Liao, Lin Du, Zezhuo Li, Zhangyating Xie, Kai Huang, Xing Lin, Zhengkun Xie, Yue Shen, Ming Chen, Tongjiang Li, Guang Feng, Yongming Sun, Long Qie, Hui Li, Fangshu Zhang, Rui Guo, Xuning Feng, Weihua Chen, Xinping Ai, Jun Lu () and Yunhui Huang ()
Additional contact information
Haijin Ji: Huazhong University of Science and Technology
Jingwei Xiang: Huazhong University of Science and Technology
Yong Li: Shanghai Institute of Space Power-Sources
Mengting Zheng: Zhejiang University
Lixia Yuan: Huazhong University of Science and Technology
Yaqi Liao: Huazhong University of Science and Technology
Lin Du: Huazhong University of Science and Technology
Zezhuo Li: Huazhong University of Science and Technology
Zhangyating Xie: Huazhong University of Science and Technology
Kai Huang: Huazhong University of Science and Technology
Xing Lin: Huazhong University of Science and Technology
Zhengkun Xie: Zhengzhou University
Yue Shen: Huazhong University of Science and Technology
Ming Chen: Huazhong University of Science and Technology
Tongjiang Li: Huazhong University of Science and Technology
Guang Feng: Huazhong University of Science and Technology
Yongming Sun: Huazhong University of Science and Technology
Long Qie: Huazhong University of Science and Technology
Hui Li: Wuhan University
Fangshu Zhang: Tsinghua University
Rui Guo: Shanghai Institute of Space Power-Sources
Xuning Feng: Tsinghua University
Weihua Chen: Zhengzhou University
Xinping Ai: Wuhan University
Jun Lu: Zhejiang University
Yunhui Huang: Huazhong University of Science and Technology

Nature, 2025, vol. 643, issue 8074, 1255-1262

Abstract: Abstract A lithium (Li)-metal anode paired with a high-nickel cathode is considered to be a combination that holds promise to surpass the 500 Wh kg−1 threshold1,2. Approaching such high energy density, electrolytes capable of stabilizing both anode and cathode interphases are of importance to secure safe and long-term cycling3,4. Although anion-derived inorganic interphases have shown remarkable success at the Li side5–7, developing intrinsic strategies to concurrently protect both electrodes remains a key challenge. Here we report a micro-emulsion strategy for electrolyte design that bypasses the Li+ solvation regulation and produces fluoride-rich interphases for both electrodes. Specifically, liquid–liquid interfacial tension between the micelles and carbonate solvents, rather than the electric field, propels the motion of fluorinated droplets towards the anode and the cathode. In this way, the interphase construction of both electrodes can be enhanced and decoupled from the solvation structure strategy. Through use of the micro-emulsion electrolyte, two pouch full cells with energy densities of 531 Wh kg−1 and 547 Wh kg−1 retain 81% and 79% of their capacity after 189 and 155 cycles, respectively. The introduction of liquid–liquid interfacial tension provides a perspective for interphase regulation and electrolyte design, and paves the way for the development of high-voltage Li-metal batteries.

Date: 2025
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DOI: 10.1038/s41586-025-09293-4

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