Silicon-based all-solid-state batteries operating free from external pressure

Abstract Silicon-based all-solid-state batteries offer high energy density and safety but face significant application challenges due to the requirement of high external pressure. In this study, a Li21Si5/Si–Li21Si5 double-layered anode is developed for all-solid-state batteries operating free from...

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Main Authors: Zhiyong Zhang, Xiuli Zhang, Yan Liu, Chaofei Lan, Xiang Han, Shanpeng Pei, Linshan Luo, Pengfei Su, Ziqi Zhang, Jingjing Liu, Zhengliang Gong, Cheng Li, Guangyang Lin, Wei Huang, Ming-Sheng Wang, Songyan Chen
Format: Article
Language:English
Published: Nature Portfolio 2025-01-01
Series:Nature Communications
Online Access:https://doi.org/10.1038/s41467-025-56366-z
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author Zhiyong Zhang
Xiuli Zhang
Yan Liu
Chaofei Lan
Xiang Han
Shanpeng Pei
Linshan Luo
Pengfei Su
Ziqi Zhang
Jingjing Liu
Zhengliang Gong
Cheng Li
Guangyang Lin
Cheng Li
Wei Huang
Ming-Sheng Wang
Songyan Chen
author_facet Zhiyong Zhang
Xiuli Zhang
Yan Liu
Chaofei Lan
Xiang Han
Shanpeng Pei
Linshan Luo
Pengfei Su
Ziqi Zhang
Jingjing Liu
Zhengliang Gong
Cheng Li
Guangyang Lin
Cheng Li
Wei Huang
Ming-Sheng Wang
Songyan Chen
author_sort Zhiyong Zhang
collection DOAJ
description Abstract Silicon-based all-solid-state batteries offer high energy density and safety but face significant application challenges due to the requirement of high external pressure. In this study, a Li21Si5/Si–Li21Si5 double-layered anode is developed for all-solid-state batteries operating free from external pressure. Under the cold-pressed sintering of Li21Si5 alloys, the anode forms a top layer (Li21Si5 layer) with mixed ionic/electronic conduction and a bottom layer (Si–Li21Si5 layer) containing a three-dimensional continuous conductive network. The resultant uniform electric field at the anode|SSE interface eliminates the need for high external pressure and simultaneously enables a twofold enhancement of the lithium-ion flux at the anode interface. Such an efficient ionic/electronic transport system also facilitates the uniform release of cycling expansion stresses from the Si particles and stabilizes bulk-phase and interfacial structure of anode. Consequently, the Li21Si5/Si–Li21Si5 anode exhibited a critical current density of 10 mA cm−2 at 45 °C with a capacity of 10 mAh cm−2. And the Li21Si5/Si–Li21Si5|Li6PS5Cl|Li3InCl6|LCO cell achieve an high initial Coulombic efficiency of (97 ± 0.7)% with areal capacity of 2.8 mAh cm−2 at 0.25 mA cm−2, as well as a low expansion rate of 14.5% after 1000 cycles at 2.5 mA cm−2.
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spelling doaj-art-a8598dbe22884afd9fbd8fde2a0b92aa2025-01-26T12:42:13ZengNature PortfolioNature Communications2041-17232025-01-0116111110.1038/s41467-025-56366-zSilicon-based all-solid-state batteries operating free from external pressureZhiyong Zhang0Xiuli Zhang1Yan Liu2Chaofei Lan3Xiang Han4Shanpeng Pei5Linshan Luo6Pengfei Su7Ziqi Zhang8Jingjing Liu9Zhengliang Gong10Cheng Li11Guangyang Lin12Cheng Li13Wei Huang14Ming-Sheng Wang15Songyan Chen16Department of Physics, Collaborative Innovation Center for Optoelectronic Semiconductors and Efficient Devices, Key Laboratory of Low Dimensional Condensed Matter Physics (Department of Education of Fujian Province), Jiujiang Research Institute, Xiamen UniversityState Key Lab of Physical Chemistry of Solid Surfaces, College of Materials, Xiamen UniversitySchool of Semiconductor Science and Technology, South China Normal UniversityDepartment of Physics, Collaborative Innovation Center for Optoelectronic Semiconductors and Efficient Devices, Key Laboratory of Low Dimensional Condensed Matter Physics (Department of Education of Fujian Province), Jiujiang Research Institute, Xiamen UniversityCollege of Materials Science and Engineering, Co-Innovation Center of Efficient Processing and Utilization of Forest Resources, Nanjing Forestry UniversityDepartment of Physics, Collaborative Innovation Center for Optoelectronic Semiconductors and Efficient Devices, Key Laboratory of Low Dimensional Condensed Matter Physics (Department of Education of Fujian Province), Jiujiang Research Institute, Xiamen UniversityDepartment of Physics, Collaborative Innovation Center for Optoelectronic Semiconductors and Efficient Devices, Key Laboratory of Low Dimensional Condensed Matter Physics (Department of Education of Fujian Province), Jiujiang Research Institute, Xiamen UniversityDepartment of Physics, Collaborative Innovation Center for Optoelectronic Semiconductors and Efficient Devices, Key Laboratory of Low Dimensional Condensed Matter Physics (Department of Education of Fujian Province), Jiujiang Research Institute, Xiamen UniversityScience and Technology on Analog Integrated Circuit LaboratoryMicrosoft Corporation, One Microsoft WayCollege of Energy, Xiamen UniversityCollege of Energy, Xiamen UniversityDepartment of Physics, Collaborative Innovation Center for Optoelectronic Semiconductors and Efficient Devices, Key Laboratory of Low Dimensional Condensed Matter Physics (Department of Education of Fujian Province), Jiujiang Research Institute, Xiamen UniversityDepartment of Physics, Collaborative Innovation Center for Optoelectronic Semiconductors and Efficient Devices, Key Laboratory of Low Dimensional Condensed Matter Physics (Department of Education of Fujian Province), Jiujiang Research Institute, Xiamen UniversityDepartment of Physics, Collaborative Innovation Center for Optoelectronic Semiconductors and Efficient Devices, Key Laboratory of Low Dimensional Condensed Matter Physics (Department of Education of Fujian Province), Jiujiang Research Institute, Xiamen UniversityDepartment of Physics, Collaborative Innovation Center for Optoelectronic Semiconductors and Efficient Devices, Key Laboratory of Low Dimensional Condensed Matter Physics (Department of Education of Fujian Province), Jiujiang Research Institute, Xiamen UniversityDepartment of Physics, Collaborative Innovation Center for Optoelectronic Semiconductors and Efficient Devices, Key Laboratory of Low Dimensional Condensed Matter Physics (Department of Education of Fujian Province), Jiujiang Research Institute, Xiamen UniversityAbstract Silicon-based all-solid-state batteries offer high energy density and safety but face significant application challenges due to the requirement of high external pressure. In this study, a Li21Si5/Si–Li21Si5 double-layered anode is developed for all-solid-state batteries operating free from external pressure. Under the cold-pressed sintering of Li21Si5 alloys, the anode forms a top layer (Li21Si5 layer) with mixed ionic/electronic conduction and a bottom layer (Si–Li21Si5 layer) containing a three-dimensional continuous conductive network. The resultant uniform electric field at the anode|SSE interface eliminates the need for high external pressure and simultaneously enables a twofold enhancement of the lithium-ion flux at the anode interface. Such an efficient ionic/electronic transport system also facilitates the uniform release of cycling expansion stresses from the Si particles and stabilizes bulk-phase and interfacial structure of anode. Consequently, the Li21Si5/Si–Li21Si5 anode exhibited a critical current density of 10 mA cm−2 at 45 °C with a capacity of 10 mAh cm−2. And the Li21Si5/Si–Li21Si5|Li6PS5Cl|Li3InCl6|LCO cell achieve an high initial Coulombic efficiency of (97 ± 0.7)% with areal capacity of 2.8 mAh cm−2 at 0.25 mA cm−2, as well as a low expansion rate of 14.5% after 1000 cycles at 2.5 mA cm−2.https://doi.org/10.1038/s41467-025-56366-z
spellingShingle Zhiyong Zhang
Xiuli Zhang
Yan Liu
Chaofei Lan
Xiang Han
Shanpeng Pei
Linshan Luo
Pengfei Su
Ziqi Zhang
Jingjing Liu
Zhengliang Gong
Cheng Li
Guangyang Lin
Cheng Li
Wei Huang
Ming-Sheng Wang
Songyan Chen
Silicon-based all-solid-state batteries operating free from external pressure
Nature Communications
title Silicon-based all-solid-state batteries operating free from external pressure
title_full Silicon-based all-solid-state batteries operating free from external pressure
title_fullStr Silicon-based all-solid-state batteries operating free from external pressure
title_full_unstemmed Silicon-based all-solid-state batteries operating free from external pressure
title_short Silicon-based all-solid-state batteries operating free from external pressure
title_sort silicon based all solid state batteries operating free from external pressure
url https://doi.org/10.1038/s41467-025-56366-z
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