The stability of the electrode-electrolyte interface in layered oxides is enhanced by electrolyte design criteria. A weakly-solvated electrolyte containing ethyl trifluoroacetate solvents with perfluorinated functional groups can restrain electrolyte decomposition and structural degradation when subjected to heat attack, exhibiting superior cycling durability at 60 °C compared to other fluorinated electrolytes.
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http://dx.doi.org/10.1039/d5cc00158g | DOI Listing |
Chem Commun (Camb)
March 2025
Siyuan Laboratory, Guangdong Provincial Engineering Technology Research Center of Vacuum Coating Technologies and New Materials, Guangdong Provincial Key Laboratory of Nanophotonic Manipulation, Department of Physics, Jinan University, Guangzhou 510632, China.
The stability of the electrode-electrolyte interface in layered oxides is enhanced by electrolyte design criteria. A weakly-solvated electrolyte containing ethyl trifluoroacetate solvents with perfluorinated functional groups can restrain electrolyte decomposition and structural degradation when subjected to heat attack, exhibiting superior cycling durability at 60 °C compared to other fluorinated electrolytes.
View Article and Find Full Text PDFAdv Mater
March 2025
Department of Chemical and Biomolecular Engineering, Korea Advanced Institute of Science and Technology (KAIST), 291 Daehak-ro Yuseong-gu, Daejeon, 34141, Republic of Korea.
The grain sizes of solid electrolyte interphase (SEI) and solvation structure of electrolytes can affect Li ion transport across SEI and control the desolvation kinetics of solvated Li ions during fast-charging of Li-ion batteries (LIBs). However, the impact of the geometric structure of SEI grains on the fast charging capability of LIBs is rarely examined. Here, the correlation between the SEI grain size and fast charging characteristics of cells is explored, and the desolvation kinetics is controlled by replacing the strongly binding ethylene carbonate (EC) solvent with a weakly binding nitrile-based solvent under fast charging conditions.
View Article and Find Full Text PDFAdv Mater
March 2025
Qingdao Industrial Energy Storage Research Institute, Qingdao Institute of Bioenergy and Bioprocess Technology, Chinese Academy of Sciences, Qingdao, 266101, P. R. China.
Multivalent-metal batteries hold tremendous promise in solving safety and sustainability problems encountered by common lithium-ion batteries, but the lack of ideal electrolyte solutions restricts their large-scale adoption. Tuning electrolyte structures with functional ingredients, especially amines/methoxy-based amines and phosphates, can revitalize multivalent-metal anodes and high-voltage cathodes in conventional electrolytes, unlocking their full potential. However, a rational and clear understanding of the implications of these ingredients, notwithstanding critically important to commercially available electrolyte design, has not been widely accepted.
View Article and Find Full Text PDFPhys Chem Chem Phys
February 2025
NISSAN ARC, Ltd., 1 Natsushima-cho, Yokosuka, Kanagawa 237-0061, Japan.
The solid electrolyte interphase (SEI) formed on the electrode in Li-ion batteries plays an important role not only in surface durability but also in charge transfer reactions. Herein, design principles for large-current batteries are presented after simulating various surface-modified graphite electrodes. Activation energies for the solvation and desolvation processes in the charge transfer reaction of the Li ion were determined at equilibrium using a hybrid method combining first-principles (density functional theory) and solution theory (reference interaction site method), in which electrochemical behaviors are well described.
View Article and Find Full Text PDFNatl Sci Rev
March 2025
Institute for Carbon Neutralization Technology, College of Chemistry and Materials Engineering, Wenzhou University, Wenzhou 325035, China.
Phosphonate-based electrolytes with the merits of low cost and intrinsic nonflammability are promising candidates to realize the safe operation of sodium-ion batteries. However, they generally suffer from poor interfacial chemistry because of the solvent-dominated solvation structure induced by the strong ion-dipole interactions between cations and phosphonate molecules. Herein, we report an electrolyte design strategy that selectively improves the competitive coordination of low-solvating-power molecules, achieving stable interfacial chemistry with a non-flammable, low-cost and fluorine-free electrolyte.
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