Large-Scale Simulation Unveiled Superior Potassium-Based Solid Electrolyte with High Ionic Conductivity and Excellent Electrochemical Stability in M_{5}YSi_{4}O_{12} (M=Li,K)
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...
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American Physical Society
2025-08-01
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| Series: | PRX Energy |
| Online Access: | http://doi.org/10.1103/8wkh-238p |
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| author | Zhao Li Jiaxiang Li Congwei Xie Keith Butler Fei Du Yu Xie |
| author_facet | Zhao Li Jiaxiang Li Congwei Xie Keith Butler Fei Du Yu Xie |
| author_sort | Zhao Li |
| collection | DOAJ |
| description | 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 K_{5}YSi_{4}O_{12} is such an outstanding electrolyte for K-ion batteries that showcases both intrinsic interfacial stability with metal anode and fast ion diffusivity. Conversely, Li_{5}YSi_{4}O_{12} only exhibits mediocre performance for Li-ion batteries. Our results show Li_{5}YSi_{4}O_{12} is thermodynamically unstable and will be reduced by the metal anode, whereas thermodynamically stable K_{5}YSi_{4}O_{12} 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 Li_{5}YSi_{4}O_{12} and K_{5}YSi_{4}O_{12}, respectively. Moreover, a significant size effect has been observed in K_{5}YSi_{4}O_{12}, 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 K_{5}YSi_{4}O_{12}. This work identifies an excellent electrolyte candidate for K-ion batteries and underscores the importance of scale in the modeling of ionic conductivity. |
| format | Article |
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| institution | DOAJ |
| issn | 2768-5608 |
| language | English |
| publishDate | 2025-08-01 |
| publisher | American Physical Society |
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| series | PRX Energy |
| spelling | doaj-art-0cb300356b5047bebbaa83daa5a5f0ff2025-08-20T03:05:50ZengAmerican Physical SocietyPRX Energy2768-56082025-08-014303300710.1103/8wkh-238pLarge-Scale Simulation Unveiled Superior Potassium-Based Solid Electrolyte with High Ionic Conductivity and Excellent Electrochemical Stability in M_{5}YSi_{4}O_{12} (M=Li,K)Zhao LiJiaxiang LiCongwei XieKeith ButlerFei DuYu XieSimultaneously 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 K_{5}YSi_{4}O_{12} is such an outstanding electrolyte for K-ion batteries that showcases both intrinsic interfacial stability with metal anode and fast ion diffusivity. Conversely, Li_{5}YSi_{4}O_{12} only exhibits mediocre performance for Li-ion batteries. Our results show Li_{5}YSi_{4}O_{12} is thermodynamically unstable and will be reduced by the metal anode, whereas thermodynamically stable K_{5}YSi_{4}O_{12} 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 Li_{5}YSi_{4}O_{12} and K_{5}YSi_{4}O_{12}, respectively. Moreover, a significant size effect has been observed in K_{5}YSi_{4}O_{12}, 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 K_{5}YSi_{4}O_{12}. This work identifies an excellent electrolyte candidate for K-ion batteries and underscores the importance of scale in the modeling of ionic conductivity.http://doi.org/10.1103/8wkh-238p |
| spellingShingle | Zhao Li Jiaxiang Li Congwei Xie Keith Butler Fei Du Yu Xie Large-Scale Simulation Unveiled Superior Potassium-Based Solid Electrolyte with High Ionic Conductivity and Excellent Electrochemical Stability in M_{5}YSi_{4}O_{12} (M=Li,K) PRX Energy |
| title | Large-Scale Simulation Unveiled Superior Potassium-Based Solid Electrolyte with High Ionic Conductivity and Excellent Electrochemical Stability in M_{5}YSi_{4}O_{12} (M=Li,K) |
| title_full | Large-Scale Simulation Unveiled Superior Potassium-Based Solid Electrolyte with High Ionic Conductivity and Excellent Electrochemical Stability in M_{5}YSi_{4}O_{12} (M=Li,K) |
| title_fullStr | Large-Scale Simulation Unveiled Superior Potassium-Based Solid Electrolyte with High Ionic Conductivity and Excellent Electrochemical Stability in M_{5}YSi_{4}O_{12} (M=Li,K) |
| title_full_unstemmed | Large-Scale Simulation Unveiled Superior Potassium-Based Solid Electrolyte with High Ionic Conductivity and Excellent Electrochemical Stability in M_{5}YSi_{4}O_{12} (M=Li,K) |
| title_short | Large-Scale Simulation Unveiled Superior Potassium-Based Solid Electrolyte with High Ionic Conductivity and Excellent Electrochemical Stability in M_{5}YSi_{4}O_{12} (M=Li,K) |
| title_sort | large scale simulation unveiled superior potassium based solid electrolyte with high ionic conductivity and excellent electrochemical stability in m 5 ysi 4 o 12 m li k |
| url | http://doi.org/10.1103/8wkh-238p |
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