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    Mesoscale engineering of ionic percolation networks in solid-state electrolytes

    Yue Zhang, Xinshui Zhang, Zeyu Wang, Tianyi Gao, Hongshen Shi, Jiameng Yu, Yihang Yang, Qiong Yuan, Wei Liu* et al.

    Yi Yu†

    • State Key Laboratory of Quantum Functional Materials, School of Physical Science and Technology, Shanghai Key Laboratory of High-resolution Electron Microscopy, ShanghaiTech University, Shanghai 201210, China

    • *Contact author: liuwei1@shanghaitech.edu.cn
    • †Contact author: yuyi1@shanghaitech.edu.cn

    Phys. Rev. B 114, 254202 – Published 4 November, 2026

    DOI: https://doi.org/10.1103/261f-bvf8

    Abstract

    Solid-state ionic conductors are pivotal for advancing energy storage technologies, yet their performance is critically governed by mesoscale structural features that influence ionic percolation pathways. In this work, random resistance model is employed to unravel the effects of mesoscopic features, including the size, shape, and alignment of grains and pores, on ionic transport percolation networks in polycrystalline ionic conductors. Our simulations reveal that larger grain sizes and vertically aligned columnar grains significantly enhance ionic conductivity by reducing percolation thresholds. Notably, vertically aligned pores further optimize percolation networks, enabling conductivity exceeding that of fully dense materials in specific configurations. By correlating simulated results with experimental data for garnet-type lithium-ion and oxygen-ion conductors, we demonstrate the model's robustness in predicting structure-property relationships. These insights establish a universal framework for designing high-performance solid electrolytes through mesoscale engineering, with broad implications for batteries, fuel cells, and beyond.

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