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,...

Full description

Bibliographic Details
Main Authors: 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
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