Towards long-life 500 Wh kg−1 lithium metal pouch cells via compact ion-pair aggregate electrolytes

Yulin Jie, Shiyang Wang, Suting Weng, Yue Liu, Ming Yang, Chao Tang, Xinpeng Li, Zhengfeng Zhang, Yuchen Zhang, Yawei Chen, Fanyang Huang, Yaolin Xu, Wanxia Li, Youzhang Guo, Zixu He, Xiaodi Ren, Yuhao Lu, Ke Yang, Saichao Cao, He Lin, Ruiguo Cao, Pengfei Yan, Tao Cheng (), Xuefeng Wang (), Shuhong Jiao () and Dongsheng Xu ()
Additional contact information
Yulin Jie: University of Science and Technology of China
Shiyang Wang: Peking University
Suting Weng: Chinese Academy of Sciences
Yue Liu: Soochow University
Ming Yang: Tianjin Institute of Power Sources
Chao Tang: University of Science and Technology of China
Xinpeng Li: University of Science and Technology of China
Zhengfeng Zhang: Beijing University of Technology
Yuchen Zhang: University of Science and Technology of China
Yawei Chen: University of Science and Technology of China
Fanyang Huang: University of Science and Technology of China
Yaolin Xu: Helmholtz-Zentrum Berlin für Materialien und Energie
Wanxia Li: University of Science and Technology of China
Youzhang Guo: University of Science and Technology of China
Zixu He: University of Science and Technology of China
Xiaodi Ren: University of Science and Technology of China
Yuhao Lu: Ningde Amperex Technology
Ke Yang: Chinese Academy of Sciences
Saichao Cao: Chinese Academy of Sciences
He Lin: Chinese Academy of Sciences
Ruiguo Cao: University of Science and Technology of China
Pengfei Yan: Beijing University of Technology
Tao Cheng: Soochow University
Xuefeng Wang: Chinese Academy of Sciences
Shuhong Jiao: University of Science and Technology of China
Dongsheng Xu: Peking University

Nature Energy, 2024, vol. 9, issue 8, 987-998

Abstract: Abstract The development of practical lithium metal cells is plagued by their limited lifespan, primarily due to the poor interfacial stability of the electrolytes. Here we present a compact ion-pair aggregate (CIPA) electrolyte that enables high-performance Li metal pouch cells under lean electrolyte conditions. The electrolyte features a unique nanometre-scale solvation structure in which ion pairs are densely packed to form large CIPAs, in contrast to conventional electrolytes that comprise small aggregates. Notably, the CIPAs facilitate fast interfacial reduction kinetics on the Li metal anode via a collective electron-transfer process, leading to the formation of a stable interface. A 505.9 Wh kg−1 Li metal pouch cell with a high-nickel-content cathode (LiNi0.905Co0.06Mn0.035O2) exhibited a 91% energy retention after 130 cycles. This work demonstrates nanostructured electrolyte design for realizing high-performance Li metal batteries. It also showcases the importance of understanding interfacial reaction mechanisms in the design and development of electrolytes.

Date: 2024
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DOI: 10.1038/s41560-024-01565-z

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