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Research Article

Insight into the influence of ether and ester electrolytes on the sodium-ion transportation kinetics for hard carbon

Xiuping YinZhaomin WangYang LiuZhixiu LuHongli LongTao LiuJiujun ZhangYufeng Zhao( )
College of Sciences & Institute for Sustainable Energy, Shanghai University, Shanghai 200444, China
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Graphical Abstract

The intrinsic mechanisms for the enhanced rate performance in ether-based electrolytes are systematically revealed through experiments and theoretical calculations. Significantly enhanced Na+ diffusion coefficient, thinner and lower impedance solid electrolyte interphase (SEI), and low desolvation energy in ether electrolytes ensure high rate capability for hard carbon (HC).

Abstract

The electrochemical performance of hard carbon (HC) materials is closely related to the electrolyte used in the sodium ion batteries (SIBs). Conventional electrolytes carbonate (EC) demonstrates low initial Columbic efficiency (ICE) and poor rate performance, which is one of the main bottlenecks that limits the practical application of HCs. Ether electrolyte (diglyme) was reported to improve the rate performance of HCs. Nevertheless, the underlying mechanism for the excellent rate capability is still lack of in-depth study. In this work, the differences of sodium-ion diffusion between ether and carbonate-base electrolytes in HCs are analyzed layer by layer. Firstly, when sodium-ions are diffused in electrolyte, the diffusion coefficient of sodium-ion in ether electrolyte is about 2.5 times higher than that in ester electrolytes by molecular dynamics (MD) simulation and experimental characterization. Furthermore, when the solvated sodium-ions are diffused into the solid electrolyte interphase (SEI) interface and the HCs material, the enhanced charge transfer kinetics (thin SEI layer (4.6 vs. 12 nm) and low RSEI (1.5 vs. 24 Ω)) at the SEI combined with low desolvation energy (0.248 eV) are responsible for high-rate performance and good cycling stability of HC in ether electrolyte. Therefore, high diffusion coefficient, low desolvation energy, and good interface are the intrinsic reasons for enhanced rate performance in ether electrolyte, which also has guiding significance for the design of other high-rate electrolytes.

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Nano Research
Pages 10922-10930
Cite this article:
Yin X, Wang Z, Liu Y, et al. Insight into the influence of ether and ester electrolytes on the sodium-ion transportation kinetics for hard carbon. Nano Research, 2023, 16(8): 10922-10930. https://doi.org/10.1007/s12274-023-5793-9
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Received: 22 March 2023
Revised: 22 April 2023
Accepted: 02 May 2023
Published: 29 June 2023
© Tsinghua University Press 2023
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