Direct calculation of effective mobile ion concentration in lithium superionic conductors

Abstract In the realm of lithium superionic conductors, pursuing higher ionic conductivity is imperative, with the variance in lithium-ion concentration playing a determining role. Due to the permanent and temporary site-blocking effects, especially at non-dilute concentrations, not all Li-ions cont...

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Main Authors: Bowei Pu, Zheyi Zou, Jinping Liu, Bing He, Dezhi Chen, Da Wang, Yue Liu, Maxim Avdeev, Siqi Shi
Format: Article
Language:English
Published: Nature Portfolio 2025-02-01
Series:npj Computational Materials
Online Access:https://doi.org/10.1038/s41524-025-01516-6
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author Bowei Pu
Zheyi Zou
Jinping Liu
Bing He
Dezhi Chen
Da Wang
Yue Liu
Maxim Avdeev
Siqi Shi
author_facet Bowei Pu
Zheyi Zou
Jinping Liu
Bing He
Dezhi Chen
Da Wang
Yue Liu
Maxim Avdeev
Siqi Shi
author_sort Bowei Pu
collection DOAJ
description Abstract In the realm of lithium superionic conductors, pursuing higher ionic conductivity is imperative, with the variance in lithium-ion concentration playing a determining role. Due to the permanent and temporary site-blocking effects, especially at non-dilute concentrations, not all Li-ions contribute to ionic conductivity. Here, we propose a strategy to directly calculate effective mobile ion concentration in which multiple-ion correlated migration is considered in the percolation analysis with the input of Li-ion distributions and hopping behavior based on kinetic Monte Carlo simulation, termed P-KMC. We provide examples of two representative lithium superionic conductors, cubic garnet-type Li x A 3 B 2O12 (0 ≤ x ≤ 9; A and B represent different cations) and perovskite-type Li x La2/3−x/3TiO3 (0 ≤ x ≤ 0.5), to demonstrate the direct dependence of the ionic conductivity on the effective mobile ion concentration. This methodology provides a robust tool to identify the optimal compositions for the highest ionic conductivity in superionic conductors.
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spelling doaj-art-b745dd5702d64794bfaf9e135063f0a42025-08-20T02:15:00ZengNature Portfolionpj Computational Materials2057-39602025-02-011111810.1038/s41524-025-01516-6Direct calculation of effective mobile ion concentration in lithium superionic conductorsBowei Pu0Zheyi Zou1Jinping Liu2Bing He3Dezhi Chen4Da Wang5Yue Liu6Maxim Avdeev7Siqi Shi8State Key Laboratory of Materials for Advanced Nuclear Energy & School of Materials Science and Engineering, Shanghai UniversitySchool of Materials Science and Engineering, Xiangtan UniversityState Key Laboratory of Materials for Advanced Nuclear Energy & School of Materials Science and Engineering, Shanghai UniversitySchool of Computer Engineering and Science, Shanghai UniversitySchool of Materials Science and Engineering, Xiangtan UniversityState Key Laboratory of Materials for Advanced Nuclear Energy & School of Materials Science and Engineering, Shanghai UniversitySchool of Computer Engineering and Science, Shanghai UniversitySchool of Chemistry, The University of SydneyState Key Laboratory of Materials for Advanced Nuclear Energy & School of Materials Science and Engineering, Shanghai UniversityAbstract In the realm of lithium superionic conductors, pursuing higher ionic conductivity is imperative, with the variance in lithium-ion concentration playing a determining role. Due to the permanent and temporary site-blocking effects, especially at non-dilute concentrations, not all Li-ions contribute to ionic conductivity. Here, we propose a strategy to directly calculate effective mobile ion concentration in which multiple-ion correlated migration is considered in the percolation analysis with the input of Li-ion distributions and hopping behavior based on kinetic Monte Carlo simulation, termed P-KMC. We provide examples of two representative lithium superionic conductors, cubic garnet-type Li x A 3 B 2O12 (0 ≤ x ≤ 9; A and B represent different cations) and perovskite-type Li x La2/3−x/3TiO3 (0 ≤ x ≤ 0.5), to demonstrate the direct dependence of the ionic conductivity on the effective mobile ion concentration. This methodology provides a robust tool to identify the optimal compositions for the highest ionic conductivity in superionic conductors.https://doi.org/10.1038/s41524-025-01516-6
spellingShingle Bowei Pu
Zheyi Zou
Jinping Liu
Bing He
Dezhi Chen
Da Wang
Yue Liu
Maxim Avdeev
Siqi Shi
Direct calculation of effective mobile ion concentration in lithium superionic conductors
npj Computational Materials
title Direct calculation of effective mobile ion concentration in lithium superionic conductors
title_full Direct calculation of effective mobile ion concentration in lithium superionic conductors
title_fullStr Direct calculation of effective mobile ion concentration in lithium superionic conductors
title_full_unstemmed Direct calculation of effective mobile ion concentration in lithium superionic conductors
title_short Direct calculation of effective mobile ion concentration in lithium superionic conductors
title_sort direct calculation of effective mobile ion concentration in lithium superionic conductors
url https://doi.org/10.1038/s41524-025-01516-6
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