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Ion‐Dipole Chemistry Drives Rapid Evolution of Li Ions Solvation Sheath in Low‐Temperature Li Batteries

Wang, Zhenxing, Sun, Zhenhua, Shi, Ying, Qi, Fulai, Gao, Xuning, Yang, Huicong, Cheng, Hui‐Ming, Li, Feng·2021·Advanced Energy Materials

DOI 10.1002/aenm.202100935

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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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A Competitive Ion-Dipole Interaction-Regulated Nonflammable Electrolyte Enables High-Energy-Density Li-Ion Batteries with Li-Rich Oxide Cathodes.
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Propylamine solvent co-intercalation in graphite electrodes for low temperature sodium-ion batteries
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Propylene Carbonate-Mediated Multisolvent Dipole Regulation Enables Wide-Temperature Batteries
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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
ORCID: Wang, Zhenxing
Sun, Zhenhua
Shi, Ying
Qi, Fulai
Yang, Huicong
Cheng, Hui‐Ming
Li, Feng
Venue: Advanced Energy Materials
Publisher: Wiley
Published: 2021-05-28
Volume: 11
Issue: 28
ISSN: 1614-6832 (ISSN-L)
1614-6840
DOI: 10.1002/aenm.202100935
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
Licence: onlinelibrary.wiley.com/termsAndConditions#vor (vor)
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 › Battery Modeling and Management
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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Ion‐Dipole Chemistry Drives Rapid Evolution of Li Ions Solvation Sheath in Low‐Temperature Li Batteries

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