Homogeneous and mechanically stable solid–electrolyte interphase enabled by trioxane-modulated electrolytes for lithium metal batteries

Qian-Kui Zhang, Xue-Qiang Zhang, Jing Wan, Nan Yao, Ting-Lu Song, Jin Xie, Li-Peng Hou, Ming-Yue Zhou, Xiang Chen, Bo-Quan Li, Rui Wen, Hong-Jie Peng, Qiang Zhang and Jia-Qi Huang ()
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Qian-Kui Zhang: Beijing Institute of Technology
Xue-Qiang Zhang: Beijing Institute of Technology
Jing Wan: Chinese Academy of Sciences
Nan Yao: Tsinghua University
Ting-Lu Song: Beijing Institute of Technology
Jin Xie: Tsinghua University
Li-Peng Hou: Tsinghua University
Ming-Yue Zhou: Tsinghua University
Xiang Chen: Tsinghua University
Bo-Quan Li: Beijing Institute of Technology
Rui Wen: Chinese Academy of Sciences
Hong-Jie Peng: University of Electronic Science and Technology of China
Qiang Zhang: Tsinghua University
Jia-Qi Huang: Beijing Institute of Technology

Nature Energy, 2023, vol. 8, issue 7, 725-735

Abstract: Abstract The solid–electrolyte interphase (SEI) in lithium (Li) metal batteries is often heterogeneous, containing a diverse range of species and has poor mechanical stability. The SEI undergoes constant cracking and reconstruction during electrochemical cycling, which is accompanied by the exhaustion of active Li and electrolytes, hindering practical applications of the batteries. Here we propose an in situ structural design of SEI to promote its homogeneity and improve its mechanical stability. A bilayer structure of SEI is tailored through trioxane-modulated electrolytes: the inner layer is dominated by LiF to improve homogeneity while the outer layer contains Li polyoxymethylene to improve mechanical stability, synergistically leading to mitigated reconstruction of SEI and reversible Li plating/stripping. The coin cell consisting of an ultrathin Li metal anode (50 μm) and a high-loading cathode (3.0 mAh cm−2)—with the tailored bilayer SEI—achieves 430 cycles tested at 1.2 mA cm−2, while the cell with an anion-derived SEI undergoes only 200 cycles under same conditions. A prototype 440 Wh kg−1 pouch cell (5.3 Ah), with a low negative/positive capacity ratio of 1.8 and lean electrolytes of 2.1 g Ah−1, achieves 130 cycles.

Date: 2023
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DOI: 10.1038/s41560-023-01275-y

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