Synergistic Anion and Solvent-Derived Interphases Enable Lithium-Ion Batteries under Extreme Conditions

Lithium-ion batteries (LIBs) face increasingly stringent demands as their application expands into new areas, including extreme temperatures and fast charging. To meet these demands, the electrolyte should enable fast lithium-ion transport and form stable interphases on electrodes simultaneously. In practice, however, improving one aspect often compromises another. For instance, the trend toward electrolytes forming anion-derived interphases typically reduces transport efficiency due to weak-solvating solvents. We propose that instead of relying on anions to form the interphase, leveraging both solvents and anions to form interphases can potentially lead to a balancing point between robust interphase formation and effective ion transport. Guided by this design principle, 2,2-difluoroethyl ethyl carbonate (DFDEC) was identified as the promising solvent. With the new electrolyte using DFDEC as the major solvent and lithium bis(fluorosulfonyl) imide (LiFSI) as the salt, graphite||LiNi<sub>0.8</sub>Mn<sub>0.1</sub>Co<sub>0.1</sub>O<sub>2</sub> (NMC811) full cells are capable of fast charging and demonstrate long-term cycling stability with a cutoff voltage of 4.5 V. Notably, the battery shows a capacity retention of 84.3% after 500 cycles with an average Coulombic efficiency (CE) as high as 99.93%. This new electrolyte also enables stable battery cycling across a wide temperature range (-20 to 60 °C), with excellent capacity retention.

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Publication Details

Journal
Journal of the American Chemical Society
Published
2024-10-25
DOI
https://doi.org/10.1021/jacs.4c07806
Citations
20
Primary Topic
Advancements in Battery Materials
Type
article
Field-Weighted Citation Impact
4.17

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article

Synergistic Anion and Solvent-Derived Interphases Enable Lithium-Ion Batteries under Extreme Conditions

Enyuan Hu, Conan Weiland, Sha Tan, Dean Yen et al.
20 citations
Journal of the American Chemical Society
Advancements in Battery Materials
4.17
article

Synergistic Anion and Solvent-Derived Interphases Enable Lithium-Ion Batteries under Extreme Conditions

Enyuan Hu, Conan Weiland, Sha Tan, Dean Yen, Nan Wang, Oleg Borodin
article en
20 citations

Abstract

Lithium-ion batteries (LIBs) face increasingly stringent demands as their application expands into new areas, including extreme temperatures and fast charging. To meet these demands, the electrolyte should enable fast lithium-ion transport and form stable interphases on electrodes simultaneously. In practice, however, improving one aspect often compromises another. For instance, the trend toward electrolytes forming anion-derived interphases typically reduces transport efficiency due to weak-solvating solvents. We propose that instead of relying on anions to form the interphase, leveraging both solvents and anions to form interphases can potentially lead to a balancing point between robust interphase formation and effective ion transport. Guided by this design principle, 2,2-difluoroethyl ethyl carbonate (DFDEC) was identified as the promising solvent. With the new electrolyte using DFDEC as the major solvent and lithium bis(fluorosulfonyl) imide (LiFSI) as the salt, graphite||LiNi<sub>0.8</sub>Mn<sub>0.1</sub>Co<sub>0.1</sub>O<sub>2</sub> (NMC811) full cells are capable of fast charging and demonstrate long-term cycling stability with a cutoff voltage of 4.5 V. Notably, the battery shows a capacity retention of 84.3% after 500 cycles with an average Coulombic efficiency (CE) as high as 99.93%. This new electrolyte also enables stable battery cycling across a wide temperature range (-20 to 60 °C), with excellent capacity retention.

Journal of the American Chemical SocietyVol. 146(44)
National Institute of Standards and Technology (US), DEVCOM Army Research Laboratory (US), Brookhaven National Laboratory (US), Battery Park (US), United States Army Combat Capabilities Development Command (US), Division of Chemistry (US), National Institute of Standards (EG), Material Measurement Laboratory (US), Measurement Specialties (Germany) (DE), Industrial Measurement Systems (United States) (US)
Vehicle Technologies Office
Affordable and clean energy
Openalex Percentile: Top 5%
Advancements in Battery Materials
4.17
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