Rapid Thermal Shutdown of Deep‐Eutectic‐Polymer Electrolyte Enabling Overheating Self‐Protection of Lithium Metal Batteries

Abstract Safety concerns and uncontrollable dendrite growths have severely impeded the advancement of lithium‐metal batteries. Herein, a safe deep‐eutectic‐polymer electrolyte with built‐in thermal shutdown capability is proposed by utilizing hydrophobic association of methylcellulose within a novel...

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Main Authors: Zengqi Zhang, Gang Li, Xiaofan Du, Lang Huang, Guohong Kang, Jianjun Zhang, Zili Cui, Tao Liu, Ling Ni, Yongcheng Jin, Guanglei Cui
Format: Article
Language:English
Published: Wiley 2024-12-01
Series:Advanced Science
Subjects:
Online Access:https://doi.org/10.1002/advs.202409628
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author Zengqi Zhang
Gang Li
Xiaofan Du
Lang Huang
Guohong Kang
Jianjun Zhang
Zili Cui
Tao Liu
Ling Ni
Yongcheng Jin
Guanglei Cui
author_facet Zengqi Zhang
Gang Li
Xiaofan Du
Lang Huang
Guohong Kang
Jianjun Zhang
Zili Cui
Tao Liu
Ling Ni
Yongcheng Jin
Guanglei Cui
author_sort Zengqi Zhang
collection DOAJ
description Abstract Safety concerns and uncontrollable dendrite growths have severely impeded the advancement of lithium‐metal batteries. Herein, a safe deep‐eutectic‐polymer electrolyte with built‐in thermal shutdown capability is proposed by utilizing hydrophobic association of methylcellulose within a novel deep‐eutectic‐solvent. Specifically, at elevated temperatures, methylcellulose chains aggregate to form dense polymer networks due to hydrophobic association and break the solvation structure equilibrium inside the deep‐eutectic system through encapsulating Li+ in polymer matrix, leading to quick solidification of the electrolyte. The solidified electrolyte obstructs Li+ transports and terminates electrochemical processes, protecting LMBs from unstoppable exothermic chain reactions. The accelerating rate calorimeter tests of 1 Ah pouch cells demonstrate that the as‐prepared electrolyte significantly improves the onset self‐heating temperature from 73 °C for conventional electrolytes to 172 °C and prolongs the thermal runaway waiting time more than 20 hours. More impressively, benefiting from its favorable electrochemical performance, this polymer electrolyte enables LiNi0.8Mn0.1Co0.1O2||Li batteries to retain 92% capacity over 200 cycles and LiFePO4||Li batteries to maintain 90% capacity after 500 cycles. This research paves a promising avenue for enhancing both the safety and electrochemical performance of high‐energy‐density LMBs.
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institution Kabale University
issn 2198-3844
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publisher Wiley
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spelling doaj-art-a0c422ab6a654bf6b007ea4100f9594b2024-12-27T13:00:47ZengWileyAdvanced Science2198-38442024-12-011148n/an/a10.1002/advs.202409628Rapid Thermal Shutdown of Deep‐Eutectic‐Polymer Electrolyte Enabling Overheating Self‐Protection of Lithium Metal BatteriesZengqi Zhang0Gang Li1Xiaofan Du2Lang Huang3Guohong Kang4Jianjun Zhang5Zili Cui6Tao Liu7Ling Ni8Yongcheng Jin9Guanglei Cui10School of Materials Science and Engineering Ocean University of China Qingdao 266100 P. R. ChinaSchool of Materials Science and Engineering Ocean University of China Qingdao 266100 P. R. ChinaQingdao Industrial Energy Storage Research Institute Qingdao Institute of Bioenergy and Bioprocess Technology Chinese Academy of Sciences Qingdao 266101 P. R. ChinaQingdao Industrial Energy Storage Research Institute Qingdao Institute of Bioenergy and Bioprocess Technology Chinese Academy of Sciences Qingdao 266101 P. R. ChinaQingdao Industrial Energy Storage Research Institute Qingdao Institute of Bioenergy and Bioprocess Technology Chinese Academy of Sciences Qingdao 266101 P. R. ChinaQingdao Industrial Energy Storage Research Institute Qingdao Institute of Bioenergy and Bioprocess Technology Chinese Academy of Sciences Qingdao 266101 P. R. ChinaQingdao Industrial Energy Storage Research Institute Qingdao Institute of Bioenergy and Bioprocess Technology Chinese Academy of Sciences Qingdao 266101 P. R. ChinaQingdao Industrial Energy Storage Research Institute Qingdao Institute of Bioenergy and Bioprocess Technology Chinese Academy of Sciences Qingdao 266101 P. R. ChinaQingdao Industrial Energy Storage Research Institute Qingdao Institute of Bioenergy and Bioprocess Technology Chinese Academy of Sciences Qingdao 266101 P. R. ChinaSchool of Materials Science and Engineering Ocean University of China Qingdao 266100 P. R. ChinaQingdao Industrial Energy Storage Research Institute Qingdao Institute of Bioenergy and Bioprocess Technology Chinese Academy of Sciences Qingdao 266101 P. R. ChinaAbstract Safety concerns and uncontrollable dendrite growths have severely impeded the advancement of lithium‐metal batteries. Herein, a safe deep‐eutectic‐polymer electrolyte with built‐in thermal shutdown capability is proposed by utilizing hydrophobic association of methylcellulose within a novel deep‐eutectic‐solvent. Specifically, at elevated temperatures, methylcellulose chains aggregate to form dense polymer networks due to hydrophobic association and break the solvation structure equilibrium inside the deep‐eutectic system through encapsulating Li+ in polymer matrix, leading to quick solidification of the electrolyte. The solidified electrolyte obstructs Li+ transports and terminates electrochemical processes, protecting LMBs from unstoppable exothermic chain reactions. The accelerating rate calorimeter tests of 1 Ah pouch cells demonstrate that the as‐prepared electrolyte significantly improves the onset self‐heating temperature from 73 °C for conventional electrolytes to 172 °C and prolongs the thermal runaway waiting time more than 20 hours. More impressively, benefiting from its favorable electrochemical performance, this polymer electrolyte enables LiNi0.8Mn0.1Co0.1O2||Li batteries to retain 92% capacity over 200 cycles and LiFePO4||Li batteries to maintain 90% capacity after 500 cycles. This research paves a promising avenue for enhancing both the safety and electrochemical performance of high‐energy‐density LMBs.https://doi.org/10.1002/advs.202409628deep‐eutectic‐polymer electrolytelithium metal batterieslong cycle lifethermal safetythermal shutdown
spellingShingle Zengqi Zhang
Gang Li
Xiaofan Du
Lang Huang
Guohong Kang
Jianjun Zhang
Zili Cui
Tao Liu
Ling Ni
Yongcheng Jin
Guanglei Cui
Rapid Thermal Shutdown of Deep‐Eutectic‐Polymer Electrolyte Enabling Overheating Self‐Protection of Lithium Metal Batteries
Advanced Science
deep‐eutectic‐polymer electrolyte
lithium metal batteries
long cycle life
thermal safety
thermal shutdown
title Rapid Thermal Shutdown of Deep‐Eutectic‐Polymer Electrolyte Enabling Overheating Self‐Protection of Lithium Metal Batteries
title_full Rapid Thermal Shutdown of Deep‐Eutectic‐Polymer Electrolyte Enabling Overheating Self‐Protection of Lithium Metal Batteries
title_fullStr Rapid Thermal Shutdown of Deep‐Eutectic‐Polymer Electrolyte Enabling Overheating Self‐Protection of Lithium Metal Batteries
title_full_unstemmed Rapid Thermal Shutdown of Deep‐Eutectic‐Polymer Electrolyte Enabling Overheating Self‐Protection of Lithium Metal Batteries
title_short Rapid Thermal Shutdown of Deep‐Eutectic‐Polymer Electrolyte Enabling Overheating Self‐Protection of Lithium Metal Batteries
title_sort rapid thermal shutdown of deep eutectic polymer electrolyte enabling overheating self protection of lithium metal batteries
topic deep‐eutectic‐polymer electrolyte
lithium metal batteries
long cycle life
thermal safety
thermal shutdown
url https://doi.org/10.1002/advs.202409628
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