Ion‐Dipole Chemistry Drives Rapid Evolution of Li Ions Solvation Sheath in Low‐Temperature Li Batteries
Abstract
Sluggish evolution of lithium ions’ solvation sheath induces large charge‐transfer barriers and high ion diffusion barriers through the passivation layer, resulting in undesirable lithium dendrite formation and capacity loss of lithium batteries, especially at low temperatures. Here, an ion‐dipole strategy by regulating the fluorination degree of solvating agents is proposed to accelerate the evolution of the Li + solvation sheath. Ethylene carbonate (EC)‐based fluorinated derivatives, fluoroethylene carbonate (FEC) and di‐fluoro ethylene carbonate (DFEC) are used as the solvating agents for a high dielectric constant. As the increase of the fluorination degree from EC to FEC and DFEC, the Li + ‐dipole interaction strength gradually decreases from 1.90 to 1.66 and 1.44 eV, respectively. Consequently, the DFEC‐based electrolyte displays six times faster ion desolvation rate than that of a non‐fluorinated EC‐based electrolyte at −20 °C. Furthermore, LiNi 0.8 Co 0.1 Mn 0.1 O 2 ||lithium cells in a DFEC‐based electrolyte retain 91% original capacity after 300 cycles at 25 °C, and 51% room‐temperature capacity at −30 °C. By bridging the gap between the ion‐dipole interactions and the evolution of Li + solvation sheath, this work provides a new technique toward rational design of electrolyte engineering for low‐temperature lithium batteries.
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Reducing the intrinsic solvating power of solvents by fluorination improves the low-temperature performance of electrolytes.
“which is another essential strategy to improve the LT performance of electrolytes by reducing the intrinsic solvating power of solvents.”
From Review on Low-Temperature Electrolytes for Lithium-Ion and Lithium Metal Batteries (2023) · cites this paper as [127]
The Li+-dipole interaction strength decreases from 1.90 to 1.66 eV and then to 1.44 eV as the fluorination degree increases from EC to FEC to DFEC.
“Experimental and calculation results demonstrated that the Li + -dipole interaction strength gradually decreases from 1.90 to 1.66 eV and then to 1.44 eV with an increase of the fluorination degree from EC to FEC and DFEC, respectively.”
From Review on Low-Temperature Electrolytes for Lithium-Ion and Lithium Metal Batteries (2023) · cites this paper as [127]
The DFEC-based electrolyte displays six times faster ion desolvation rates than the EC-based electrolyte at -20 °C.
“the DFEC-based electrolyte displays six times faster ion desolvation rates than that of the EC-based electrolyte at -20 °C.”
From Review on Low-Temperature Electrolytes for Lithium-Ion and Lithium Metal Batteries (2023) · cites this paper as [127]
NMC811-Li cells with DFEC-based electrolyte displayed better fast-charge capability and long-term cyclability from -30 to 25 °C compared to cells with EC-based electrolyte.
“NMC811-Li cells with the DFECbased electrolyte displayed better fast-charge capability and long-term cyclability in the temperature range from -30 to 25 °C compared to that with the EC-based electrolyte.”
From Review on Low-Temperature Electrolytes for Lithium-Ion and Lithium Metal Batteries (2023) · cites this paper as [127]
Fluorination of a polar solvent enhances its electronegativity and reduces its polarity.
“The fluorination of polar solvent could enhance the electronegativity and reduce the polarity”
From Review on Low-Temperature Electrolytes for Lithium-Ion and Lithium Metal Batteries (2023) · cites this paper as [127]
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- Authors
- Wang, Z., Sun, Z., Shi, Y., Qi, F., Gao, X., Yang, H., Cheng, H., & Li, F.
- Affiliations
- University of Science and Technology of China (CN)
- Chinese Academy of Sciences (CN)
- Corresponding author
- Sun, Zhenhua
- Li, Feng
- Venue
- Advanced Energy Materials
- Publisher
- Wiley
- Published
- 2021-05-28
- Volume
- 11
- Issue
- 28
- ISSN
- 1614-6832 (ISSN-L)
- 1614-6840
- OpenAlex
- W3172441039
- Cited by
- 202
- References
- 53
- Citations by year
- 2026: 25 · 2025: 45 · 2024: 46 · 2023: 47 · 2022: 34 · 2021: 5
- FWCI
- 9.71
- Type
- journal article
- Language
- en
- Open access
- closed
- Locations
- Advanced Energy Materials (publishedVersion)
- Funders
- Tsinghua University
- National Natural Science Foundation of China (52020105010, 51927803, 51972313, 51525206, 52072378)
- Liaoning Revitalization Talents Program (XLYC1908015)
- Youth Innovation Promotion Association of the Chinese Academy of Sciences (Y201942)
- Topics
- Physical Sciences › Engineering › Electrical and Electronic Engineering › Advanced Battery Materials and Technologies
- Physical Sciences › Engineering › Electrical and Electronic Engineering › Advancements in Battery Materials
- Physical Sciences › Engineering › Automotive Engineering › Advanced Battery Technologies Research
- Keywords
- ion-dipole interactions, fluoroethylene carbonate, ethylene carbonate, electrolyte engineering, ion desolvation, lithium dendrite suppression, capacity retention, LiNi0.8Co0.1Mn0.1O2 cathode
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