Accelerated Defluorination Kinetics for an Ultrathin Solid–Electrolyte Interphase in Durable Lithium Metal Batteries

The cycle life of lithium (Li) metal batteries is plagued by the rapid depletion of electrolyte and Li inventory due to the continuous formation of a massive, thick solid-electrolyte interphase (SEI). Here, <i>in situ</i> generation of an ultrathin SEI is proposed by accelerating defluorination kinetics of the electrolyte to retrench the amount of electrolyte and Li inventory in SEI formation for durable batteries. The ultrathin SEI is generated in a dimethoxy(dimethyl)silane (DMDMS)-based electrolyte. Compared with the dispersed contact ion pairs in routine electrolytes, DMDMS, with both ultrahigh solubility of Li salts and weak solvating power, is favorable for the formation of joint aggregates in the electrolyte. The joint aggregates exhibit a fast defluorination rate, inducing uniform and compact nucleation sites on the Li metal surface. The compact nucleation sites grow simultaneously and subsequently come into contact with each other. This process rapidly passivates the exposed anode surface and facilitates the formation of an ultrathin SEI. The prototype pouch cell (≥500 Wh kg<sup>-1</sup>) with the ultrathin SEI achieves 190 cycles and can operate at -30 °C with 66% energy retention. This work reveals the formation mechanism of the SEI and demonstrates the potential of meticulous SEI engineering in the development of durable Li metal batteries.

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Publication Details

Journal
Journal of the American Chemical Society
Published
2025-12-19
DOI
https://doi.org/10.1021/jacs.5c16009
Citations
2
Primary Topic
Advanced Battery Materials and Technologies
Type
article
Field-Weighted Citation Impact
1.46
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article

Accelerated Defluorination Kinetics for an Ultrathin Solid–Electrolyte Interphase in Durable Lithium Metal Batteries

Wenjun Feng, Qiankui Zhang, Shu‐Yu Sun, Rui Wen et al.
2 citations
Journal of the American Chemical Society
Advanced Battery Materials and Technologies
1.46
article

Accelerated Defluorination Kinetics for an Ultrathin Solid–Electrolyte Interphase in Durable Lithium Metal Batteries

Wenjun Feng, Qiankui Zhang, Shu‐Yu Sun, Rui Wen, Tao Cheng, Peiping Yu, Jia‐Qi Huang, Bo‐Quan Li, Hong‐Jie Peng, Ya-Nan Wang, Xin‐Bing Cheng, Xiao-Qing Ding, Nan Yao, Qiang Zhang, Yuan Li, Zheng Zhao, Xue‐Qiang Zhang, Yue Zhao, Jialin Li
article en
2 citations

Abstract

The cycle life of lithium (Li) metal batteries is plagued by the rapid depletion of electrolyte and Li inventory due to the continuous formation of a massive, thick solid-electrolyte interphase (SEI). Here, <i>in situ</i> generation of an ultrathin SEI is proposed by accelerating defluorination kinetics of the electrolyte to retrench the amount of electrolyte and Li inventory in SEI formation for durable batteries. The ultrathin SEI is generated in a dimethoxy(dimethyl)silane (DMDMS)-based electrolyte. Compared with the dispersed contact ion pairs in routine electrolytes, DMDMS, with both ultrahigh solubility of Li salts and weak solvating power, is favorable for the formation of joint aggregates in the electrolyte. The joint aggregates exhibit a fast defluorination rate, inducing uniform and compact nucleation sites on the Li metal surface. The compact nucleation sites grow simultaneously and subsequently come into contact with each other. This process rapidly passivates the exposed anode surface and facilitates the formation of an ultrathin SEI. The prototype pouch cell (≥500 Wh kg<sup>-1</sup>) with the ultrathin SEI achieves 190 cycles and can operate at -30 °C with 66% energy retention. This work reveals the formation mechanism of the SEI and demonstrates the potential of meticulous SEI engineering in the development of durable Li metal batteries.

Journal of the American Chemical SocietyVol. 148(7)
Beijing Institute of Technology (CN), University of Electronic Science and Technology of China (CN), Chinese Academy of Sciences (CN), Soochow University (CN), Ministry of Education (RO), Huaneng Clean Energy Research Institute (CN), Beijing National Laboratory for Molecular Sciences (CN), Carbon180 (US), University of Chinese Academy of Sciences (CN), Nano Carbon (Poland) (PL), Southeast University (CN), Tsinghua University (CN)
Openalex Percentile: Top 14%
Advanced Battery Materials and Technologies
1.46
DOISourceOpenAlex
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