External Li supply reshapes Li deficiency and lifetime limit of batteries

Shu Chen, Guanbin Wu, Haibo Jiang, Jifeng Wang, Tiantian Chen, Chenyang Han, Wenwen Wang, Rongchen Yang, Jiahua Zhao, Zhihang Tang, Xiaocheng Gong, Chuanfa Li, Mengyao Zhu, Kun Zhang, Yifei Xu, Ying Wang, Zhe Hu, Peining Chen, Bingjie Wang, Kai Zhang, Yongyao Xia, Huisheng Peng () and Yue Gao ()
Additional contact information
Shu Chen: Fudan University
Guanbin Wu: Fudan University
Haibo Jiang: Fudan University
Jifeng Wang: Fudan University
Tiantian Chen: Fudan University
Chenyang Han: Fudan University
Wenwen Wang: Fudan University
Rongchen Yang: Fudan University
Jiahua Zhao: Nankai University
Zhihang Tang: Hunan Institute of Engineering
Xiaocheng Gong: Fudan University
Chuanfa Li: Fudan University
Mengyao Zhu: Fudan University
Kun Zhang: Fudan University
Yifei Xu: Fudan University
Ying Wang: Fudan University
Zhe Hu: Shenzhen University
Peining Chen: Fudan University
Bingjie Wang: Fudan University
Kai Zhang: Nankai University
Yongyao Xia: Fudan University
Huisheng Peng: Fudan University
Yue Gao: Fudan University

Nature, 2025, vol. 638, issue 8051, 676-683

Abstract: Abstract Lithium (Li) ions are central to the energy storing functionality of rechargeable batteries1. Present technology relies on sophisticated Li-inclusive electrode materials to provide Li ions and exactingly protect them to ensure a decent lifetime2. Li-deficient materials are thus excluded from battery design, and the battery fails when active Li ions are consumed3. Our study breaks this limit by means of a cell-level Li supply strategy. This involves externally adding an organic Li salt into an assembled cell, which decomposes during cell formation, liberating Li ions and expelling organic ligands as gases. This non-invasive and rapid process preserves cell integrity without necessitating disassembly. We leveraged machine learning to discover such functional salts and identified lithium trifluoromethanesulfinate (LiSO2CF3) with optimal electrochemical activity, potential, product formation, electrolyte solubility and specific capacity. As a proof-of-concept, we demonstrated a 3.0 V, 1,192 Wh kg−1 Li-free cathode, chromium oxide, in the anode-less cell, as well as an organic sulfurized polyacrylonitrile cathode incorporated in a 388 Wh kg−1 pouch cell with a 440-cycle life. These systems exhibit improved energy density, enhanced sustainability and reduced cost compared with conventional Li-ion batteries. Furthermore, the lifetime of commercial LiFePO4 batteries was extended by at least an order of magnitude. With repeated external Li supplies, a commercial graphite|LiFePO4 cell displayed a capacity retention of 96.0% after 11,818 cycles.

Date: 2025
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DOI: 10.1038/s41586-024-08465-y

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