HybridSolvent Coupled with Dual-Salt ElectrolyteEnables High-Performance Lithium–Metal Batteries

Lithium–metal batteries (LMBs) are widely recognized as the next-generation energy storage technology due to their high energy density, while their commercialization is hindered by the low Coulombic efficiency and uncontrolled Li dendrite growth. To address these challenges, an anion-rich solvation structure is achieved by a hybrid solvent coupled with a dual-salt electrolyte. The strongly coordinating DTA binds tightly to Li<sup>+</sup> in the first solvation sheath, while the weakly coordinating FEC occupies the second solvation shell. Moreover, FEC, with a weak coordinating ability, allows TFSI<sup>–</sup> and DFOB<sup>–</sup> to enter the primary solvation sheath. The anion-derived SEIs exhibit enhanced mechanical strength and ionic conductivity, leading to accelerated Li<sup>+</sup> transport kinetics and inhibited Li dendrite growth. As a result, the Li||Cu half-cell employing a hybrid solvent coupled with a dual-salt electrolyte delivers an average Aurbach Coulombic efficiency of 99.0%. Moreover, the Li||LiNi<sub>0.8</sub>Co<sub>0.1</sub>Mn<sub>0.1</sub>O<sub>2</sub> battery exhibits robust capacity retention of 90.8% over 300 cycles, demonstrating the viability of hybrid solvent coupled with dual-salt electrolyte in practical LMBs.

Publication Details

Journal
Figshare
Published
2025-02-06
DOI
https://doi.org/10.1021/acsami.4c21546.s001
Primary Topic
Advanced Battery Materials and Technologies
Type
article
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article

HybridSolvent Coupled with Dual-Salt ElectrolyteEnables High-Performance Lithium–Metal Batteries

Figshare
Advanced Battery Materials and Technologies
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HybridSolvent Coupled with Dual-Salt ElectrolyteEnables High-Performance Lithium–Metal Batteries

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Abstract

Lithium–metal batteries (LMBs) are widely recognized as the next-generation energy storage technology due to their high energy density, while their commercialization is hindered by the low Coulombic efficiency and uncontrolled Li dendrite growth. To address these challenges, an anion-rich solvation structure is achieved by a hybrid solvent coupled with a dual-salt electrolyte. The strongly coordinating DTA binds tightly to Li<sup>+</sup> in the first solvation sheath, while the weakly coordinating FEC occupies the second solvation shell. Moreover, FEC, with a weak coordinating ability, allows TFSI<sup>–</sup> and DFOB<sup>–</sup> to enter the primary solvation sheath. The anion-derived SEIs exhibit enhanced mechanical strength and ionic conductivity, leading to accelerated Li<sup>+</sup> transport kinetics and inhibited Li dendrite growth. As a result, the Li||Cu half-cell employing a hybrid solvent coupled with a dual-salt electrolyte delivers an average Aurbach Coulombic efficiency of 99.0%. Moreover, the Li||LiNi<sub>0.8</sub>Co<sub>0.1</sub>Mn<sub>0.1</sub>O<sub>2</sub> battery exhibits robust capacity retention of 90.8% over 300 cycles, demonstrating the viability of hybrid solvent coupled with dual-salt electrolyte in practical LMBs.

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HybridSolvent Coupled with Dual-Salt ElectrolyteEnables High-Performance Lithium–Metal Batteries · Figshare (2025) | TGRS Research Map | TGRS