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<p>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>i.e</i>., 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||LiCoO<sub>2</sub> with 90% capacity retention after 600 cycles at 0.2 C/0.5 C charge/discharge rate. Notably, Cu||LiNi<sub>0.5</sub>Co<sub>0.2</sub>Mn<sub>0.3</sub>O<sub>2</sub> 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.</p>

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

  • 期刊论文

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  • 发表日期：

    2025年5月20日

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  • 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,
  • Xiulin Fan

摘要

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.