A path towards high lithium-metal electrode coulombic efficiency based on electrolyte interaction motif descriptor
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 physicoche...
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| Main Authors: | , , , , , , , , , , , , , , , , |
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| Format: | Article |
| Language: | English |
| Published: |
Nature Portfolio
2025-05-01
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| Series: | Nature Communications |
| Online Access: | https://doi.org/10.1038/s41467-025-59955-0 |
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| Summary: | 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. |
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| ISSN: | 2041-1723 |