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A path towards high lithium-metal electrode coulombic efficiency based on electrolyte interaction motif descriptor

Ruhong Li, Xiaoteng Huang, Haikuo Zhang, Jinze Wang, Yingzhu Fan, Yiqiang Huang, Jia Liu, Ming Yang, Yuan Yu, Xuezhang Xiao, Yuanzhong Tan, Hao Bin Wu, Liwu Fan, Tao Deng, Lixin Chen, Yanbin Shen and Xiulin Fan ()
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Ruhong Li: Zhejiang University
Xiaoteng Huang: Zhejiang University
Haikuo Zhang: Zhejiang University
Jinze Wang: Zhejiang University
Yingzhu Fan: Chinese Academy of Sciences
Yiqiang Huang: Zhejiang University
Jia Liu: Zhejiang University
Ming Yang: Tianjin Institute of Power Sources
Yuan Yu: Zhejiang Sci-Tech University
Xuezhang Xiao: Zhejiang University
Yuanzhong Tan: Zhejiang Xinan Chemical Industrial Group Co. Ltd
Hao Bin Wu: Zhejiang University
Liwu Fan: Zhejiang University
Tao Deng: Shanghai Jiao Tong University
Lixin Chen: Zhejiang University
Yanbin Shen: Chinese Academy of Sciences
Xiulin Fan: Zhejiang University

Nature Communications, 2025, vol. 16, issue 1, 1-14

Abstract: Abstract The fundamental interactions and the as-derived microstructures among electrolyte components play a pivotal role in determining the bulk and interfacial properties of the electrolytes. However, the complex structure-property relationships remain elusive, leading to uncontrollable physicochemical characteristics of electrolytes and unsatisfied battery performance. Herein, we propose two interaction motif descriptors to quantify ion-solvent interactions spanning electrostatic to dispersion regimes. These descriptors are highly relevant to salt dissolution, phase miscibility, and electrode-electrolyte interface chemistries. Guided by the principle of minimizing ion-solvent and solvent-solvent interactions while ensuring sufficient salt dissociation, a representative electrolyte, i.e., lithium bis(fluorosulfonyl)imide dissolved in trimethyl methoxysilane and 1,3,5-trifluorobenzene with a molar ratio of 1:2.5:3.0, is designed, which achieves ~99.7% (±0.2%) Li plating/stripping Coulombic efficiency and endows 4.5 V Li||LiCoO2 with 90% capacity retention after 600 cycles at 0.2 C/0.5 C charge/discharge rate. Notably, Cu||LiNi0.5Co0.2Mn0.3O2 pouch cells with this electrolyte sustain over 100 stable cycles. By establishing quantitative relationships between interaction motifs and electrolyte functionalities, this work provides a universal framework for rational electrolyte design, paving the way for highly reversible lithium metal batteries.

Date: 2025
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DOI: 10.1038/s41467-025-59955-0

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