Promoting high-voltage stability through local lattice distortion of halide solid electrolytes
Abstract Stable solid electrolytes are essential to high-safety and high-energy-density lithium batteries, especially for applications with high-voltage cathodes. In such conditions, solid electrolytes may experience severe oxidation, decomposition, and deactivation during charging at high voltages,...
Main Authors: | , , , , , , , , , , , , , , , , |
---|---|
Format: | Article |
Language: | English |
Published: |
Nature Portfolio
2024-02-01
|
Series: | Nature Communications |
Online Access: | https://doi.org/10.1038/s41467-024-45864-1 |
_version_ | 1797274124330991616 |
---|---|
author | Zhenyou Song Tengrui Wang Hua Yang Wang Hay Kan Yuwei Chen Qian Yu Likuo Wang Yini Zhang Yiming Dai Huaican Chen Wen Yin Takashi Honda Maxim Avdeev Henghui Xu Jiwei Ma Yunhui Huang Wei Luo |
author_facet | Zhenyou Song Tengrui Wang Hua Yang Wang Hay Kan Yuwei Chen Qian Yu Likuo Wang Yini Zhang Yiming Dai Huaican Chen Wen Yin Takashi Honda Maxim Avdeev Henghui Xu Jiwei Ma Yunhui Huang Wei Luo |
author_sort | Zhenyou Song |
collection | DOAJ |
description | Abstract Stable solid electrolytes are essential to high-safety and high-energy-density lithium batteries, especially for applications with high-voltage cathodes. In such conditions, solid electrolytes may experience severe oxidation, decomposition, and deactivation during charging at high voltages, leading to inadequate cycling performance and even cell failure. Here, we address the high-voltage limitation of halide solid electrolytes by introducing local lattice distortion to confine the distribution of Cl−, which effectively curbs kinetics of their oxidation. The confinement is realized by substituting In with multiple elements in Li3InCl6 to give a high-entropy Li2.75Y0.16Er0.16Yb0.16In0.25Zr0.25Cl6. Meanwhile, the lattice distortion promotes longer Li-Cl bonds, facilitating favorable activation of Li+. Our results show that this high-entropy halide electrolyte boosts the cycle stability of all-solid-state battery by 250% improvement over 500 cycles. In particular, the cell provides a higher discharge capacity of 185 mAh g−1 by increasing the charge cut-off voltage to 4.6 V at a small current rate of 0.2 C, which is more challenging to electrolytes|cathode stability. These findings deepen our understanding of high-entropy materials, advancing their use in energy-related applications. |
first_indexed | 2024-03-07T14:53:52Z |
format | Article |
id | doaj.art-c2b86d31795f4780a4aab46fa5d9d7a3 |
institution | Directory Open Access Journal |
issn | 2041-1723 |
language | English |
last_indexed | 2024-03-07T14:53:52Z |
publishDate | 2024-02-01 |
publisher | Nature Portfolio |
record_format | Article |
series | Nature Communications |
spelling | doaj.art-c2b86d31795f4780a4aab46fa5d9d7a32024-03-05T19:33:01ZengNature PortfolioNature Communications2041-17232024-02-011511910.1038/s41467-024-45864-1Promoting high-voltage stability through local lattice distortion of halide solid electrolytesZhenyou Song0Tengrui Wang1Hua Yang2Wang Hay Kan3Yuwei Chen4Qian Yu5Likuo Wang6Yini Zhang7Yiming Dai8Huaican Chen9Wen Yin10Takashi Honda11Maxim Avdeev12Henghui Xu13Jiwei Ma14Yunhui Huang15Wei Luo16Institute of New Energy for Vehicles, School of Materials Science and Engineering, Tongji UniversityInstitute of New Energy for Vehicles, School of Materials Science and Engineering, Tongji UniversitySpallation Neutron Source Science CenterSpallation Neutron Source Science CenterInstitute of New Energy for Vehicles, School of Materials Science and Engineering, Tongji UniversityInstitute of New Energy for Vehicles, School of Materials Science and Engineering, Tongji UniversityInstitute of New Energy for Vehicles, School of Materials Science and Engineering, Tongji UniversityInstitute of New Energy for Vehicles, School of Materials Science and Engineering, Tongji UniversityInstitute of New Energy for Vehicles, School of Materials Science and Engineering, Tongji UniversitySpallation Neutron Source Science CenterSpallation Neutron Source Science CenterInstitute of Materials Structure Science, High Energy Accelerator Research Organization (KEK)Australian Nuclear Science and Technology Organisation (ANSTO)State Key Laboratory of Material Processing and Die & Mould Technology, School of Materials Science and Engineering, Huazhong University of Science and TechnologyInstitute of New Energy for Vehicles, School of Materials Science and Engineering, Tongji UniversityState Key Laboratory of Material Processing and Die & Mould Technology, School of Materials Science and Engineering, Huazhong University of Science and TechnologyInstitute of New Energy for Vehicles, School of Materials Science and Engineering, Tongji UniversityAbstract Stable solid electrolytes are essential to high-safety and high-energy-density lithium batteries, especially for applications with high-voltage cathodes. In such conditions, solid electrolytes may experience severe oxidation, decomposition, and deactivation during charging at high voltages, leading to inadequate cycling performance and even cell failure. Here, we address the high-voltage limitation of halide solid electrolytes by introducing local lattice distortion to confine the distribution of Cl−, which effectively curbs kinetics of their oxidation. The confinement is realized by substituting In with multiple elements in Li3InCl6 to give a high-entropy Li2.75Y0.16Er0.16Yb0.16In0.25Zr0.25Cl6. Meanwhile, the lattice distortion promotes longer Li-Cl bonds, facilitating favorable activation of Li+. Our results show that this high-entropy halide electrolyte boosts the cycle stability of all-solid-state battery by 250% improvement over 500 cycles. In particular, the cell provides a higher discharge capacity of 185 mAh g−1 by increasing the charge cut-off voltage to 4.6 V at a small current rate of 0.2 C, which is more challenging to electrolytes|cathode stability. These findings deepen our understanding of high-entropy materials, advancing their use in energy-related applications.https://doi.org/10.1038/s41467-024-45864-1 |
spellingShingle | Zhenyou Song Tengrui Wang Hua Yang Wang Hay Kan Yuwei Chen Qian Yu Likuo Wang Yini Zhang Yiming Dai Huaican Chen Wen Yin Takashi Honda Maxim Avdeev Henghui Xu Jiwei Ma Yunhui Huang Wei Luo Promoting high-voltage stability through local lattice distortion of halide solid electrolytes Nature Communications |
title | Promoting high-voltage stability through local lattice distortion of halide solid electrolytes |
title_full | Promoting high-voltage stability through local lattice distortion of halide solid electrolytes |
title_fullStr | Promoting high-voltage stability through local lattice distortion of halide solid electrolytes |
title_full_unstemmed | Promoting high-voltage stability through local lattice distortion of halide solid electrolytes |
title_short | Promoting high-voltage stability through local lattice distortion of halide solid electrolytes |
title_sort | promoting high voltage stability through local lattice distortion of halide solid electrolytes |
url | https://doi.org/10.1038/s41467-024-45864-1 |
work_keys_str_mv | AT zhenyousong promotinghighvoltagestabilitythroughlocallatticedistortionofhalidesolidelectrolytes AT tengruiwang promotinghighvoltagestabilitythroughlocallatticedistortionofhalidesolidelectrolytes AT huayang promotinghighvoltagestabilitythroughlocallatticedistortionofhalidesolidelectrolytes AT wanghaykan promotinghighvoltagestabilitythroughlocallatticedistortionofhalidesolidelectrolytes AT yuweichen promotinghighvoltagestabilitythroughlocallatticedistortionofhalidesolidelectrolytes AT qianyu promotinghighvoltagestabilitythroughlocallatticedistortionofhalidesolidelectrolytes AT likuowang promotinghighvoltagestabilitythroughlocallatticedistortionofhalidesolidelectrolytes AT yinizhang promotinghighvoltagestabilitythroughlocallatticedistortionofhalidesolidelectrolytes AT yimingdai promotinghighvoltagestabilitythroughlocallatticedistortionofhalidesolidelectrolytes AT huaicanchen promotinghighvoltagestabilitythroughlocallatticedistortionofhalidesolidelectrolytes AT wenyin promotinghighvoltagestabilitythroughlocallatticedistortionofhalidesolidelectrolytes AT takashihonda promotinghighvoltagestabilitythroughlocallatticedistortionofhalidesolidelectrolytes AT maximavdeev promotinghighvoltagestabilitythroughlocallatticedistortionofhalidesolidelectrolytes AT henghuixu promotinghighvoltagestabilitythroughlocallatticedistortionofhalidesolidelectrolytes AT jiweima promotinghighvoltagestabilitythroughlocallatticedistortionofhalidesolidelectrolytes AT yunhuihuang promotinghighvoltagestabilitythroughlocallatticedistortionofhalidesolidelectrolytes AT weiluo promotinghighvoltagestabilitythroughlocallatticedistortionofhalidesolidelectrolytes |