Constructing Dissolution–Resistant Interphases for Long‐Life Sodium‐Ion Batteries at Elevated Temperatures
Abstract Rechargeable sodium‐ion batteries (SIBs) utilizing NaPF6‐carbonate electrolytes consistently exhibit unsatisfactory cycle life at elevated temperatures, posing a significant challenge for their large‐scale commercialization. This is mainly caused by the instability of interphase layers at e...
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2025-07-01
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Online Access: | https://doi.org/10.1002/advs.202502860 |
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author | Wenting Deng Xiaofan Du Gaojie Xu Shitao Wang Li Du Tiantian Dong Rongxian Wu Chuanchuan Li Zhaolin Lv Jiangwei Ju Xinhong Zhou Guanglei Cui |
author_facet | Wenting Deng Xiaofan Du Gaojie Xu Shitao Wang Li Du Tiantian Dong Rongxian Wu Chuanchuan Li Zhaolin Lv Jiangwei Ju Xinhong Zhou Guanglei Cui |
author_sort | Wenting Deng |
collection | DOAJ |
description | Abstract Rechargeable sodium‐ion batteries (SIBs) utilizing NaPF6‐carbonate electrolytes consistently exhibit unsatisfactory cycle life at elevated temperatures, posing a significant challenge for their large‐scale commercialization. This is mainly caused by the instability of interphase layers at elevated temperatures, especially the high solubility of interphase components (especially NaF) in carbonate solvents. In this study, a novel additive of sodium difluorobis(oxalato) phosphate (NaDFBOP) is synthesized and introduced into NaPF6‐carbonate electrolytes to enhance the cycle life of commercial SIBs composed of NaNi1/3Fe1/3Mn1/3O2 (NFM) cathode and hard carbon (HC) anode, particularly at 50 °C. Specifically, the NaDFBOP enables NFM/HC SIBs to retain 85.45% of initial capacity after 1000 cycles at 30 °C and 90.76% after 500 cycles at 50 °C. Theoretical calculations reveal that DFBOP⁻ anions enter the first solvation shell of Na+, and NaDFBOP exhibits a strong propensity for decomposition. Characterizations suggest that NaDFBOP favors the formation of dissolution–resistant robust interphase layers enriched of dissolution‐resistant oxalate‐containing species and inorganic NaF, which have strong mutual binding energy. This work underscores the critical importance of designing functional additives and constructing dissolution‐resistant robust interphases to enhance the elevated temperature cycle life of SIBs. |
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spelling | doaj-art-a8fc8ee1e6e240b88dd9ed85fdd3f9e82025-07-17T11:30:47ZengWileyAdvanced Science2198-38442025-07-011227n/an/a10.1002/advs.202502860Constructing Dissolution–Resistant Interphases for Long‐Life Sodium‐Ion Batteries at Elevated TemperaturesWenting Deng0Xiaofan Du1Gaojie Xu2Shitao Wang3Li Du4Tiantian Dong5Rongxian Wu6Chuanchuan Li7Zhaolin Lv8Jiangwei Ju9Xinhong Zhou10Guanglei Cui11College of Chemistry and Molecular Engineering Qingdao University of Science and Technology Qingdao 266042 ChinaQingdao Industrial Energy Storage Research Institute Qingdao Institute of Bioenergy and Bioprocess Technology Chinese Academy of Science Qingdao 266101 ChinaQingdao Industrial Energy Storage Research Institute Qingdao Institute of Bioenergy and Bioprocess Technology Chinese Academy of Science Qingdao 266101 ChinaQingdao Industrial Energy Storage Research Institute Qingdao Institute of Bioenergy and Bioprocess Technology Chinese Academy of Science Qingdao 266101 ChinaQingdao Industrial Energy Storage Research Institute Qingdao Institute of Bioenergy and Bioprocess Technology Chinese Academy of Science Qingdao 266101 ChinaQingdao Industrial Energy Storage Research Institute Qingdao Institute of Bioenergy and Bioprocess Technology Chinese Academy of Science Qingdao 266101 ChinaQingdao Industrial Energy Storage Research Institute Qingdao Institute of Bioenergy and Bioprocess Technology Chinese Academy of Science Qingdao 266101 ChinaQingdao Industrial Energy Storage Research Institute Qingdao Institute of Bioenergy and Bioprocess Technology Chinese Academy of Science Qingdao 266101 ChinaQingdao Industrial Energy Storage Research Institute Qingdao Institute of Bioenergy and Bioprocess Technology Chinese Academy of Science Qingdao 266101 ChinaQingdao Industrial Energy Storage Research Institute Qingdao Institute of Bioenergy and Bioprocess Technology Chinese Academy of Science Qingdao 266101 ChinaCollege of Chemistry and Molecular Engineering Qingdao University of Science and Technology Qingdao 266042 ChinaQingdao Industrial Energy Storage Research Institute Qingdao Institute of Bioenergy and Bioprocess Technology Chinese Academy of Science Qingdao 266101 ChinaAbstract Rechargeable sodium‐ion batteries (SIBs) utilizing NaPF6‐carbonate electrolytes consistently exhibit unsatisfactory cycle life at elevated temperatures, posing a significant challenge for their large‐scale commercialization. This is mainly caused by the instability of interphase layers at elevated temperatures, especially the high solubility of interphase components (especially NaF) in carbonate solvents. In this study, a novel additive of sodium difluorobis(oxalato) phosphate (NaDFBOP) is synthesized and introduced into NaPF6‐carbonate electrolytes to enhance the cycle life of commercial SIBs composed of NaNi1/3Fe1/3Mn1/3O2 (NFM) cathode and hard carbon (HC) anode, particularly at 50 °C. Specifically, the NaDFBOP enables NFM/HC SIBs to retain 85.45% of initial capacity after 1000 cycles at 30 °C and 90.76% after 500 cycles at 50 °C. Theoretical calculations reveal that DFBOP⁻ anions enter the first solvation shell of Na+, and NaDFBOP exhibits a strong propensity for decomposition. Characterizations suggest that NaDFBOP favors the formation of dissolution–resistant robust interphase layers enriched of dissolution‐resistant oxalate‐containing species and inorganic NaF, which have strong mutual binding energy. This work underscores the critical importance of designing functional additives and constructing dissolution‐resistant robust interphases to enhance the elevated temperature cycle life of SIBs.https://doi.org/10.1002/advs.202502860carbonate electrolytedissolution–resistant interphaseelevated temperaturefunctional additivesodium‐ion batteries |
spellingShingle | Wenting Deng Xiaofan Du Gaojie Xu Shitao Wang Li Du Tiantian Dong Rongxian Wu Chuanchuan Li Zhaolin Lv Jiangwei Ju Xinhong Zhou Guanglei Cui Constructing Dissolution–Resistant Interphases for Long‐Life Sodium‐Ion Batteries at Elevated Temperatures Advanced Science carbonate electrolyte dissolution–resistant interphase elevated temperature functional additive sodium‐ion batteries |
title | Constructing Dissolution–Resistant Interphases for Long‐Life Sodium‐Ion Batteries at Elevated Temperatures |
title_full | Constructing Dissolution–Resistant Interphases for Long‐Life Sodium‐Ion Batteries at Elevated Temperatures |
title_fullStr | Constructing Dissolution–Resistant Interphases for Long‐Life Sodium‐Ion Batteries at Elevated Temperatures |
title_full_unstemmed | Constructing Dissolution–Resistant Interphases for Long‐Life Sodium‐Ion Batteries at Elevated Temperatures |
title_short | Constructing Dissolution–Resistant Interphases for Long‐Life Sodium‐Ion Batteries at Elevated Temperatures |
title_sort | constructing dissolution resistant interphases for long life sodium ion batteries at elevated temperatures |
topic | carbonate electrolyte dissolution–resistant interphase elevated temperature functional additive sodium‐ion batteries |
url | https://doi.org/10.1002/advs.202502860 |
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