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Large-Scale Simulation Unveiled Superior Potassium-Based Solid Electrolyte with High Ionic Conductivity and Excellent Electrochemical Stability in M5YSi4O12 (M=Li,K)

Zhao Li1,*, Jiaxiang Li1,*, Congwei Xie2,†, Keith Butler3, Fei Du4, and Yu Xie1,4,‡

  • 1Key Laboratory of Material Simulation Methods and Software of Ministry of Education, College of Physics, Jilin University, Changchun 130012, China
  • 2Research Center for Crystal Materials, State Key Laboratory of Functional Materials and Devices for Special Environmental Conditions, Xinjiang Key Laboratory of Functional Crystal Materials, Xinjiang Technical Institute of Physics and Chemistry, Chinese Academy of Sciences, 40-1 South Beijing Road, Urumqi 830011, China
  • 3Department of Chemistry, University College London, Gordon Street, London WC1H 0AJ, United Kingdom
  • 4Key Laboratory of Physics and Technology for Advanced Batteries of Ministry of Education, College of Physics, Jilin University, Changchun 130012, China

  • *These authors contributed equally to this work.
  • †Contact author: cwxie@ms.xjb.ac.cn
  • ‡Contact author: xieyu@jlu.edu.cn
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PRX Energy 4, 033007 – Published 14 August, 2025

DOI: https://doi.org/10.1103/8wkh-238p

Abstract

Simultaneously achieving interfacial stability and high room-temperature ionic conductivity (≥10−3 S/cm) in solid-state electrolytes is one of the most significant challenges in the development of all-solid-state batteries. In this study, by combining first-principles simulations and large-scale machine-learning molecular dynamics modeling, we demonstrate K5YSi4O12 is such an outstanding electrolyte for K-ion batteries that showcases both intrinsic interfacial stability with metal anode and fast ion diffusivity. Conversely, Li5YSi4O12 only exhibits mediocre performance for Li-ion batteries. Our results show Li5YSi4O12 is thermodynamically unstable and will be reduced by the metal anode, whereas thermodynamically stable K5YSi4O12 presents a wide electrochemical stability window of 0.00–3.27 V versus K/K+, suggesting it is stable in contact with potassium metal. The predicted ionic conductivity is 0.43 and 3.63 mS/cm for Li5YSi4O12 and K5YSi4O12, respectively. Moreover, a significant size effect has been observed in K5YSi4O12, where the accurate ionic conductivity can only be obtained through large-scale simulations. Further analysis reveals low energy barrier and long hopping distance are responsible for the higher ionic conductivity in K5YSi4O12. This work identifies an excellent electrolyte candidate for K-ion batteries and underscores the importance of scale in the modeling of ionic conductivity.

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Developing advanced solid electrolytes with both high ionic conductivity and electrochemical stability remains a key challenge for next-generation all-solid-state batteries. Here, by combining first-principles calculations with large-scale machine learning simulations, the authors demonstrate that K5YSi4O12 exhibits promise as a solid electrolyte. This potassium-based material maintains remarkable stability against potassium metal, with a wide electrochemical stability window of 0.00-3.27 V, and achieves an ionic conductivity of 3.63 mS/cm. Importantly, these simulations reveal clear size-dependent behavior, with ionic conductivity converging as simulation scales increase. These findings not only highlight K5YSi4O12 as a promising solid electrolyte for safe, high-performance potassium-ion batteries but also emphasize the crucial importance of large-scale simulations in accurately predicting materials' properties.

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PRX Energy 4, 033007– Published 14 August, 2025
  • Received 15 January 2025
  • Revised 29 June 2025
  • Accepted 8 July 2025
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Published by the American Physical Society under the terms of the Creative Commons Attribution 4.0 International license. Further distribution of this work must maintain attribution to the author(s) and the published article's title, journal citation, and DOI.

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