Comprehensive Study of Li Deposition and Solid Electrolyte Cracking by Integrating Simulation and Experimental Data

Abstract Lithium (Li) penetration into solid‐state electrolytes (SE) is a major cause of lithium‐metal solid‐state battery (LMSSB) failure. However, no single model fully explains experimental phenomena, and many simulation‐based conclusions lack validation or contradict experimental results, hinder...

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Main Authors: Chen Lin, Haihui Ruan, Ming‐Sheng Wang
Format: Article
Language:English
Published: Wiley 2025-07-01
Series:Advanced Science
Subjects:
Online Access:https://doi.org/10.1002/advs.202501434
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author Chen Lin
Haihui Ruan
Ming‐Sheng Wang
author_facet Chen Lin
Haihui Ruan
Ming‐Sheng Wang
author_sort Chen Lin
collection DOAJ
description Abstract Lithium (Li) penetration into solid‐state electrolytes (SE) is a major cause of lithium‐metal solid‐state battery (LMSSB) failure. However, no single model fully explains experimental phenomena, and many simulation‐based conclusions lack validation or contradict experimental results, hindering the understanding of failure mechanisms. This study integrates simulation and experimental data to investigate Li deposition and SE cracking, introducing a unified phase‐field (PF) model. Unlike existing models, it accounts for mechanical constraints, solid–solid contact, and large‐strain mechano‐chemical coupling. It also distinguishes Li penetration from SE cracking, as short‐circuiting and cracking do not occur simultaneously. Additionally, crack initiation follows the pressurized cracking model, while propagation occurs through a wedge‐shaped opening. A counterintuitive approach to extending LMSSB lifespan is to reduce the mechanical constraints of SE rather than decreasing defect size or increasing SE hardness and toughness, provided that good contact is maintained between the electrode and SE. This is because minimizing mechanical constraints alters the Li deposition mode, preventing rapid Li eruption in cracks.
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spelling doaj-art-b2d30028cbc44bb7b52ddfa9d38a9a432025-08-20T03:15:35ZengWileyAdvanced Science2198-38442025-07-011225n/an/a10.1002/advs.202501434Comprehensive Study of Li Deposition and Solid Electrolyte Cracking by Integrating Simulation and Experimental DataChen Lin0Haihui Ruan1Ming‐Sheng Wang2Sino‐French Institute of Nuclear Engineering and Technology Sun Yat‐Sen University Zhuhai 519000 ChinaDepartment of Mechanical Engineering The Hong Kong Polytechnic University Hung Hom Kowloon Hong Kong 999077 ChinaState Key Laboratory of Physical Chemistry of Solid Surfaces College of Materials Xiamen University Xiamen 361000 ChinaAbstract Lithium (Li) penetration into solid‐state electrolytes (SE) is a major cause of lithium‐metal solid‐state battery (LMSSB) failure. However, no single model fully explains experimental phenomena, and many simulation‐based conclusions lack validation or contradict experimental results, hindering the understanding of failure mechanisms. This study integrates simulation and experimental data to investigate Li deposition and SE cracking, introducing a unified phase‐field (PF) model. Unlike existing models, it accounts for mechanical constraints, solid–solid contact, and large‐strain mechano‐chemical coupling. It also distinguishes Li penetration from SE cracking, as short‐circuiting and cracking do not occur simultaneously. Additionally, crack initiation follows the pressurized cracking model, while propagation occurs through a wedge‐shaped opening. A counterintuitive approach to extending LMSSB lifespan is to reduce the mechanical constraints of SE rather than decreasing defect size or increasing SE hardness and toughness, provided that good contact is maintained between the electrode and SE. This is because minimizing mechanical constraints alters the Li deposition mode, preventing rapid Li eruption in cracks.https://doi.org/10.1002/advs.202501434crackingdepositionintegrating simulation and experimental datamechanical constraint
spellingShingle Chen Lin
Haihui Ruan
Ming‐Sheng Wang
Comprehensive Study of Li Deposition and Solid Electrolyte Cracking by Integrating Simulation and Experimental Data
Advanced Science
cracking
deposition
integrating simulation and experimental data
mechanical constraint
title Comprehensive Study of Li Deposition and Solid Electrolyte Cracking by Integrating Simulation and Experimental Data
title_full Comprehensive Study of Li Deposition and Solid Electrolyte Cracking by Integrating Simulation and Experimental Data
title_fullStr Comprehensive Study of Li Deposition and Solid Electrolyte Cracking by Integrating Simulation and Experimental Data
title_full_unstemmed Comprehensive Study of Li Deposition and Solid Electrolyte Cracking by Integrating Simulation and Experimental Data
title_short Comprehensive Study of Li Deposition and Solid Electrolyte Cracking by Integrating Simulation and Experimental Data
title_sort comprehensive study of li deposition and solid electrolyte cracking by integrating simulation and experimental data
topic cracking
deposition
integrating simulation and experimental data
mechanical constraint
url https://doi.org/10.1002/advs.202501434
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AT haihuiruan comprehensivestudyoflidepositionandsolidelectrolytecrackingbyintegratingsimulationandexperimentaldata
AT mingshengwang comprehensivestudyoflidepositionandsolidelectrolytecrackingbyintegratingsimulationandexperimentaldata