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Anion-reinforced solvation structure favors the formation of inorganic-rich robust electrode-electrolyte interface, which endows fast ion transport and high strength modulus to enable improved electrochemical performance. However, such a unique solvation structure inevitably injures the ionic conductivity of electrolytes and limits the fast-charging performance. Herein, a trade-off in tuning anion-reinforced solvation structure and high ionic conductivity is realized by the entropy-assisted hybrid ester-ether electrolyte. Anion-reinforced solvation sheath with more anions occupying the inner Na shell is constructed by introducing the weakly coordinated ether tetrahydrofuran into the commonly used ester-based electrolyte, which merits the accelerated desolvation energy and gradient inorganic-rich electrode-electrolyte interface. The improved ionic conductivity is attributed to the weakly diverse solvation structures induced by entropy effect. These enable the enhanced rate performance and cycling stability of Prussian blue||hard carbon full cells with high electrode mass loading. More importantly, the practical application of the designed electrolyte was further demonstrated by industry-level 18650 cylindrical cells.
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http://dx.doi.org/10.1002/anie.202410494 | DOI Listing |
J Am Chem Soc
August 2025
Institute for Carbon Neutralization Technology, College of Chemistry and Materials Engineering, Wenzhou University, Wenzhou, Zhejiang 325035, China.
Wide-temperature sodium-ion batteries (SIBs) are considered promising candidates for large-scale energy storage systems under extreme temperature conditions. However, SIBs generally suffer from an unstable electrode-electrolyte interface (EEI) at high temperature and sluggish interfacial kinetics at low temperature, resulting in poor temperature tolerance with fast capacity degradation. Herein, a weakly coordinated carboxylate ester cosolvent, methyl butyrate, is employed to modulate the ion-dipole interactions in fluorine-free ester-based electrolyte for the anion-reinforced solvation chemistry.
View Article and Find Full Text PDFACS Appl Mater Interfaces
June 2025
School of Materials and Energy, University of Electronic Science and Technology of China, Chengdu 611731, China.
Pyrite FeS, recognized as a promising conversion-type cathode material for high-energy-density batteries, encounters a rapid decline in capacity due to the polysulfide shuttle effect. To tackle these challenges, this study introduces a nonflammable locally concentrated ionic liquid electrolyte (LCILE) composed of lithium bis(fluorosulfonyl)imide (LiFSI), 1-vinylpropyl-3-methylimidazolium bis(trifluoromethylsulfonyl)imide (AMImTFSI), and 1,1,2,2-tetrafluoroethyl-2,2,3,3-tetrafluoropropyl ether (TTE). This electrolyte manifests a tailored solvation structure with FSI-TFSI dual-anion-dominated aggregates (AGGs), which effectively mitigates the shuttle effect of polysulfides and fosters the formation of a robust dual-anion-derived cathode-electrolyte interphase (CEI) on the FeS cathode.
View Article and Find Full Text PDFChem Sci
March 2025
School of Chemical Engineering, Sichuan University Chengdu 610065 P. R. China
Poly(vinylidene fluoride) (PVDF)-based solid-state electrolytes (SSEs) have been considered promising candidates for advanced Li metal batteries due to their adequate mechanical strength and acceptable thermal stability. However, the poor compatibility between residual solvent and Li metal inevitably leads to fast capacity decay. Herein, we propose a multifunctional cation-anchor strategy to regulate solvation chemistry in PVDF-based SSEs to boost the electrochemical performance of Li metal batteries.
View Article and Find Full Text PDFAngew Chem Int Ed Engl
March 2025
State Key Laboratory of Reliability and Intelligence of Electrical Equipment, School of Materials Science and Engineering, Hebei University of Technology, Tianjin, 300401, China.
Low-concentration electrolytes (LCEs) have attracted great attention due to their cost effectiveness and low viscosity, but suffer undesired organic-rich interfacial chemistry and poor oxidative stability. Herein, a unique latent solvent, 1,2-dibutoxyethane (DBE), is proposed to manipulate the anion-reinforced solvation sheath and construct a robust inorganic-rich interface in a 0.5 M electrolyte.
View Article and Find Full Text PDFAngew Chem Int Ed Engl
October 2024
Institute for Carbon Neutralization Technology, College of Chemistry and Materials Engineering, Wenzhou University, Wenzhou, Zhejiang, 325035, China.
Anion-reinforced solvation structure favors the formation of inorganic-rich robust electrode-electrolyte interface, which endows fast ion transport and high strength modulus to enable improved electrochemical performance. However, such a unique solvation structure inevitably injures the ionic conductivity of electrolytes and limits the fast-charging performance. Herein, a trade-off in tuning anion-reinforced solvation structure and high ionic conductivity is realized by the entropy-assisted hybrid ester-ether electrolyte.
View Article and Find Full Text PDF