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Unraveling electrolyte solvation architectures for high-performance lithium-ion batteries

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Abstract

The design of advanced electrolytes hinges critically on a comprehensive comprehension of lithium-ion migration mechanisms within these electrochemical systems. Fluorination generally improves the stability and reduces the reactivity of organic compounds, making them potentially suitable for use in harsh conditions such as those found in a battery electrolyte. However, the specific properties, such as the solvation power, diffusivity, ion mobility, and so forth, would depend on the exact nature and extent of the fluorination. In this work, we introduce a theoretical framework designed to facilitate the autonomous creation of electrolyte molecular structures and craft methodologies to compute transport coefficients, providing a physical interpretation of fluoride systems. Taking fluorinated-1,2-diethoxyethanes as electrolyte solvents, we present and analyze the relationship between the electronic properties and atomic structures, and further correlate these properties to the transport coefficients, resulting in a good alignment with the experimental diffusion behaviors and Li-solvation structures. The insights derived from this research contribute to the methodological basis for high-throughput evaluation of prospective electrolyte systems, and consequently, propose strategic directions for the improvement of electrochemical cycle characteristics. This comprehensive exploration of the transport mechanisms enhances our understanding, offering avenues for further advancements in the field of lithium-ion battery technology.

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Authors and Affiliations

  1. School of Materials Science and Engineering, Tongji University, Shanghai, 201804, China

    MengHao Yang

  2. Department of Nuclear Science and Engineering, Massachusetts Institute of Technology, Cambridge, Massachusetts, 02139, USA

    Zhe Shi

  3. School of Materials Science and Engineering, Beijing Institute of Technology, Beijing, 100081, China

    ZhiYuan He & Dan Wang

Authors
  1. MengHao Yang
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  2. Zhe Shi
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  3. ZhiYuan He
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  4. Dan Wang
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Corresponding author

Correspondence to Dan Wang.

Additional information

The Density Functional Theory (DFT) calculation conducted in this study was executed using the Quantum Espresso (QE) software on the Materials Square platform. This cloud-based computational platform was used as part of the International Computational Competition organized by Virtual Lab Inc. in 2022. We also had the technical guidance of Dr. Mosab Banisalman from Virtual Lab Inc. during this process. This work was supported by the National Natural Science Foundation of China (Grant No. 52302302), the National Key R&D Program of China (Grant No. 2022YFE0208000), the Fundamental Research Funds for the Central Universities, and the Special Funds of the Tongji University for “Sino-German Cooperation 2.0 Strategy”. We also gratefully acknowledge HZWTECH for providing computation facilities.

Supporting Information

The supporting information is available online at tech.scichina.com and link.springer.com. The supporting materials are published as submitted, without typesetting or editing. The responsibility for scientific accuracy and content remains entirely with the authors.

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Yang, M., Shi, Z., He, Z. et al. Unraveling electrolyte solvation architectures for high-performance lithium-ion batteries. Sci. China Technol. Sci. 67, 958–964 (2024). https://doi.org/10.1007/s11431-023-2494-9

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  • DOI: https://doi.org/10.1007/s11431-023-2494-9

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