Intrinsically Nonflammable Ionic Liquid‐Based Localized Highly Concentrated Electrolytes Enable High‐Performance Li‐Metal Batteries

The development of high‐performance Li‐metal batteries (LMBs) requires advanced electrolytes that simultaneously possess high safety, high ionic conductivity, wide electrochemical window, and good ability to suppress Li dendrite growth. Herein an intrinsically nonflammable ionic liquid‐based localiz...

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Veröffentlicht in:Advanced energy materials 2021-05, Vol.11 (17), p.n/a
Hauptverfasser: Wang, Zhicheng, Zhang, Fengrui, Sun, Yiyang, Zheng, Lei, Shen, Yanbin, Fu, Daosong, Li, Wanfei, Pan, Anran, Wang, Lei, Xu, Jingjing, Hu, Jianchen, Wu, Xiaodong
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container_issue 17
container_start_page
container_title Advanced energy materials
container_volume 11
creator Wang, Zhicheng
Zhang, Fengrui
Sun, Yiyang
Zheng, Lei
Shen, Yanbin
Fu, Daosong
Li, Wanfei
Pan, Anran
Wang, Lei
Xu, Jingjing
Hu, Jianchen
Wu, Xiaodong
description The development of high‐performance Li‐metal batteries (LMBs) requires advanced electrolytes that simultaneously possess high safety, high ionic conductivity, wide electrochemical window, and good ability to suppress Li dendrite growth. Herein an intrinsically nonflammable ionic liquid‐based localized highly concentrated electrolyte (LHCE) composed of lithium bis(fluorosulfonyl)imide (LiFSI) salt, N‐methyl‐N‐propyl‐piperidinium bis(fluorosulfonyl)imide ([PP13][FSI]) as ionic liquid solvent, and 1,1,2,2‐tetrafluoroethyl‐2,2,3,3‐tetrafluoropropylether (HFE) as diluent solvent is designed. The introduction of HFE greatly decreases the viscosity and cost of the pure ionic liquid electrolyte, improves its ionic conductivity, and enhances its ability to wet the separator surface. The Li+ solvation structure, Li deposition behavior, and formation of the solid electrolyte interphase (SEI) layer in LHCE are systematically investigated by using Raman spectroscopy, theoretical simulations, scanning electron microscopy, and X‐ray photoelectron spectroscopy. A rational mechanism is suggested for the stable SEI formation and the homogeneous Li deposition behavior. Due to its excellent ability to suppress Li dendrites, the LHCE exhibits a high average Coulombic efficiency (99.4% over 800 cycles in the Cu/Li cell), extremely stable cycling performance (10 mA cm−2 over 5000 cycles in the Li/Li symmetric cell), and excellent cycling performance and rate capability in the LMB systems of LiFePO4 (LFP)/Li and LFP/Li@Cu. An intrinsically nonflammable localized highly concentrated electrolyte (LHCE) containing ionic liquid solvent (IL) and HFE diluent solvent is reported. The introduction of HFE greatly decreases the viscosity and cost of pure IL electrolyte, improves its ionic conductivity and its ability to wet the separator surface. Arising from homogeneous Li deposition behavior, the LHCE shows excellent cell performance in Li‐metal batteries.
doi_str_mv 10.1002/aenm.202003752
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Herein an intrinsically nonflammable ionic liquid‐based localized highly concentrated electrolyte (LHCE) composed of lithium bis(fluorosulfonyl)imide (LiFSI) salt, N‐methyl‐N‐propyl‐piperidinium bis(fluorosulfonyl)imide ([PP13][FSI]) as ionic liquid solvent, and 1,1,2,2‐tetrafluoroethyl‐2,2,3,3‐tetrafluoropropylether (HFE) as diluent solvent is designed. The introduction of HFE greatly decreases the viscosity and cost of the pure ionic liquid electrolyte, improves its ionic conductivity, and enhances its ability to wet the separator surface. The Li+ solvation structure, Li deposition behavior, and formation of the solid electrolyte interphase (SEI) layer in LHCE are systematically investigated by using Raman spectroscopy, theoretical simulations, scanning electron microscopy, and X‐ray photoelectron spectroscopy. A rational mechanism is suggested for the stable SEI formation and the homogeneous Li deposition behavior. Due to its excellent ability to suppress Li dendrites, the LHCE exhibits a high average Coulombic efficiency (99.4% over 800 cycles in the Cu/Li cell), extremely stable cycling performance (10 mA cm−2 over 5000 cycles in the Li/Li symmetric cell), and excellent cycling performance and rate capability in the LMB systems of LiFePO4 (LFP)/Li and LFP/Li@Cu. An intrinsically nonflammable localized highly concentrated electrolyte (LHCE) containing ionic liquid solvent (IL) and HFE diluent solvent is reported. The introduction of HFE greatly decreases the viscosity and cost of pure IL electrolyte, improves its ionic conductivity and its ability to wet the separator surface. Arising from homogeneous Li deposition behavior, the LHCE shows excellent cell performance in Li‐metal batteries.</description><identifier>ISSN: 1614-6832</identifier><identifier>EISSN: 1614-6840</identifier><identifier>DOI: 10.1002/aenm.202003752</identifier><language>eng</language><publisher>Weinheim: Wiley Subscription Services, Inc</publisher><subject>Cycles ; Dendritic structure ; Deposition ; Electrolytes ; Ion currents ; Ionic liquids ; Ions ; Lithium ; li‐metal batteries ; localized highly concentrated electrolytes ; nonflammable electrolytes ; Photoelectrons ; Raman spectroscopy ; safe electrolytes ; Separators ; Solid electrolytes ; Solvation ; Solvents ; Spectrum analysis</subject><ispartof>Advanced energy materials, 2021-05, Vol.11 (17), p.n/a</ispartof><rights>2021 Wiley‐VCH GmbH</rights><lds50>peer_reviewed</lds50><woscitedreferencessubscribed>false</woscitedreferencessubscribed><citedby>FETCH-LOGICAL-c3562-60f4ab0d67146c3805799b6f99b2dcaac69a4e2a3eecf074f858de70f81fc17a3</citedby><cites>FETCH-LOGICAL-c3562-60f4ab0d67146c3805799b6f99b2dcaac69a4e2a3eecf074f858de70f81fc17a3</cites><orcidid>0000-0002-1050-7660</orcidid></display><links><openurl>$$Topenurl_article</openurl><openurlfulltext>$$Topenurlfull_article</openurlfulltext><thumbnail>$$Tsyndetics_thumb_exl</thumbnail><linktopdf>$$Uhttps://onlinelibrary.wiley.com/doi/pdf/10.1002%2Faenm.202003752$$EPDF$$P50$$Gwiley$$H</linktopdf><linktohtml>$$Uhttps://onlinelibrary.wiley.com/doi/full/10.1002%2Faenm.202003752$$EHTML$$P50$$Gwiley$$H</linktohtml><link.rule.ids>314,780,784,1416,27915,27916,45565,45566</link.rule.ids></links><search><creatorcontrib>Wang, Zhicheng</creatorcontrib><creatorcontrib>Zhang, Fengrui</creatorcontrib><creatorcontrib>Sun, Yiyang</creatorcontrib><creatorcontrib>Zheng, Lei</creatorcontrib><creatorcontrib>Shen, Yanbin</creatorcontrib><creatorcontrib>Fu, Daosong</creatorcontrib><creatorcontrib>Li, Wanfei</creatorcontrib><creatorcontrib>Pan, Anran</creatorcontrib><creatorcontrib>Wang, Lei</creatorcontrib><creatorcontrib>Xu, Jingjing</creatorcontrib><creatorcontrib>Hu, Jianchen</creatorcontrib><creatorcontrib>Wu, Xiaodong</creatorcontrib><title>Intrinsically Nonflammable Ionic Liquid‐Based Localized Highly Concentrated Electrolytes Enable High‐Performance Li‐Metal Batteries</title><title>Advanced energy materials</title><description>The development of high‐performance Li‐metal batteries (LMBs) requires advanced electrolytes that simultaneously possess high safety, high ionic conductivity, wide electrochemical window, and good ability to suppress Li dendrite growth. Herein an intrinsically nonflammable ionic liquid‐based localized highly concentrated electrolyte (LHCE) composed of lithium bis(fluorosulfonyl)imide (LiFSI) salt, N‐methyl‐N‐propyl‐piperidinium bis(fluorosulfonyl)imide ([PP13][FSI]) as ionic liquid solvent, and 1,1,2,2‐tetrafluoroethyl‐2,2,3,3‐tetrafluoropropylether (HFE) as diluent solvent is designed. The introduction of HFE greatly decreases the viscosity and cost of the pure ionic liquid electrolyte, improves its ionic conductivity, and enhances its ability to wet the separator surface. The Li+ solvation structure, Li deposition behavior, and formation of the solid electrolyte interphase (SEI) layer in LHCE are systematically investigated by using Raman spectroscopy, theoretical simulations, scanning electron microscopy, and X‐ray photoelectron spectroscopy. A rational mechanism is suggested for the stable SEI formation and the homogeneous Li deposition behavior. Due to its excellent ability to suppress Li dendrites, the LHCE exhibits a high average Coulombic efficiency (99.4% over 800 cycles in the Cu/Li cell), extremely stable cycling performance (10 mA cm−2 over 5000 cycles in the Li/Li symmetric cell), and excellent cycling performance and rate capability in the LMB systems of LiFePO4 (LFP)/Li and LFP/Li@Cu. An intrinsically nonflammable localized highly concentrated electrolyte (LHCE) containing ionic liquid solvent (IL) and HFE diluent solvent is reported. The introduction of HFE greatly decreases the viscosity and cost of pure IL electrolyte, improves its ionic conductivity and its ability to wet the separator surface. Arising from homogeneous Li deposition behavior, the LHCE shows excellent cell performance in Li‐metal batteries.</description><subject>Cycles</subject><subject>Dendritic structure</subject><subject>Deposition</subject><subject>Electrolytes</subject><subject>Ion currents</subject><subject>Ionic liquids</subject><subject>Ions</subject><subject>Lithium</subject><subject>li‐metal batteries</subject><subject>localized highly concentrated electrolytes</subject><subject>nonflammable electrolytes</subject><subject>Photoelectrons</subject><subject>Raman spectroscopy</subject><subject>safe electrolytes</subject><subject>Separators</subject><subject>Solid electrolytes</subject><subject>Solvation</subject><subject>Solvents</subject><subject>Spectrum analysis</subject><issn>1614-6832</issn><issn>1614-6840</issn><fulltext>true</fulltext><rsrctype>article</rsrctype><creationdate>2021</creationdate><recordtype>article</recordtype><recordid>eNqFkD1PwzAURSMEEhV0ZY7E3OKPfI5tFWiltjDAHL06z-DKiVs7FQoTKxu_kV-CS1EZ8WA_PZ1zLd0guKJkSAlhN4BNPWSEEcLTmJ0EPZrQaJBkETk9zpydB33n1sSfKKeE817wMWtaqxqnBGjdhUvTSA11DSuN4cw0SoRztd2p6uv9cwwOq3BuPKne_DRVzy9emZhGoA-B1u8KjaK1RncturBofmL2nNcf0Epja_C0z_SLBbagwzG0LVqF7jI4k6Ad9n_fi-DptnicTAfz-7vZZDQfCB4nbJAQGcGKVElKo0TwjMRpnq8S6S9WCQCR5BAhA44oJEkjmcVZhSmRGZWCpsAvgutD7saa7Q5dW67Nzjb-y5LFjLGcs4x4anighDXOWZTlxqoabFdSUu4bL_eNl8fGvZAfhFelsfuHLkfFcvHnfgMFkIox</recordid><startdate>20210501</startdate><enddate>20210501</enddate><creator>Wang, Zhicheng</creator><creator>Zhang, Fengrui</creator><creator>Sun, Yiyang</creator><creator>Zheng, Lei</creator><creator>Shen, Yanbin</creator><creator>Fu, Daosong</creator><creator>Li, Wanfei</creator><creator>Pan, Anran</creator><creator>Wang, Lei</creator><creator>Xu, Jingjing</creator><creator>Hu, Jianchen</creator><creator>Wu, Xiaodong</creator><general>Wiley Subscription Services, Inc</general><scope>AAYXX</scope><scope>CITATION</scope><scope>7SP</scope><scope>7TB</scope><scope>8FD</scope><scope>F28</scope><scope>FR3</scope><scope>H8D</scope><scope>L7M</scope><orcidid>https://orcid.org/0000-0002-1050-7660</orcidid></search><sort><creationdate>20210501</creationdate><title>Intrinsically Nonflammable Ionic Liquid‐Based Localized Highly Concentrated Electrolytes Enable High‐Performance Li‐Metal Batteries</title><author>Wang, Zhicheng ; Zhang, Fengrui ; Sun, Yiyang ; Zheng, Lei ; Shen, Yanbin ; Fu, Daosong ; Li, Wanfei ; Pan, Anran ; Wang, Lei ; Xu, Jingjing ; Hu, Jianchen ; Wu, Xiaodong</author></sort><facets><frbrtype>5</frbrtype><frbrgroupid>cdi_FETCH-LOGICAL-c3562-60f4ab0d67146c3805799b6f99b2dcaac69a4e2a3eecf074f858de70f81fc17a3</frbrgroupid><rsrctype>articles</rsrctype><prefilter>articles</prefilter><language>eng</language><creationdate>2021</creationdate><topic>Cycles</topic><topic>Dendritic structure</topic><topic>Deposition</topic><topic>Electrolytes</topic><topic>Ion currents</topic><topic>Ionic liquids</topic><topic>Ions</topic><topic>Lithium</topic><topic>li‐metal batteries</topic><topic>localized highly concentrated electrolytes</topic><topic>nonflammable electrolytes</topic><topic>Photoelectrons</topic><topic>Raman spectroscopy</topic><topic>safe electrolytes</topic><topic>Separators</topic><topic>Solid electrolytes</topic><topic>Solvation</topic><topic>Solvents</topic><topic>Spectrum analysis</topic><toplevel>peer_reviewed</toplevel><toplevel>online_resources</toplevel><creatorcontrib>Wang, Zhicheng</creatorcontrib><creatorcontrib>Zhang, Fengrui</creatorcontrib><creatorcontrib>Sun, Yiyang</creatorcontrib><creatorcontrib>Zheng, Lei</creatorcontrib><creatorcontrib>Shen, Yanbin</creatorcontrib><creatorcontrib>Fu, Daosong</creatorcontrib><creatorcontrib>Li, Wanfei</creatorcontrib><creatorcontrib>Pan, Anran</creatorcontrib><creatorcontrib>Wang, Lei</creatorcontrib><creatorcontrib>Xu, Jingjing</creatorcontrib><creatorcontrib>Hu, Jianchen</creatorcontrib><creatorcontrib>Wu, Xiaodong</creatorcontrib><collection>CrossRef</collection><collection>Electronics &amp; 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Herein an intrinsically nonflammable ionic liquid‐based localized highly concentrated electrolyte (LHCE) composed of lithium bis(fluorosulfonyl)imide (LiFSI) salt, N‐methyl‐N‐propyl‐piperidinium bis(fluorosulfonyl)imide ([PP13][FSI]) as ionic liquid solvent, and 1,1,2,2‐tetrafluoroethyl‐2,2,3,3‐tetrafluoropropylether (HFE) as diluent solvent is designed. The introduction of HFE greatly decreases the viscosity and cost of the pure ionic liquid electrolyte, improves its ionic conductivity, and enhances its ability to wet the separator surface. The Li+ solvation structure, Li deposition behavior, and formation of the solid electrolyte interphase (SEI) layer in LHCE are systematically investigated by using Raman spectroscopy, theoretical simulations, scanning electron microscopy, and X‐ray photoelectron spectroscopy. A rational mechanism is suggested for the stable SEI formation and the homogeneous Li deposition behavior. Due to its excellent ability to suppress Li dendrites, the LHCE exhibits a high average Coulombic efficiency (99.4% over 800 cycles in the Cu/Li cell), extremely stable cycling performance (10 mA cm−2 over 5000 cycles in the Li/Li symmetric cell), and excellent cycling performance and rate capability in the LMB systems of LiFePO4 (LFP)/Li and LFP/Li@Cu. An intrinsically nonflammable localized highly concentrated electrolyte (LHCE) containing ionic liquid solvent (IL) and HFE diluent solvent is reported. The introduction of HFE greatly decreases the viscosity and cost of pure IL electrolyte, improves its ionic conductivity and its ability to wet the separator surface. Arising from homogeneous Li deposition behavior, the LHCE shows excellent cell performance in Li‐metal batteries.</abstract><cop>Weinheim</cop><pub>Wiley Subscription Services, Inc</pub><doi>10.1002/aenm.202003752</doi><tpages>8</tpages><orcidid>https://orcid.org/0000-0002-1050-7660</orcidid></addata></record>
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source Wiley Online Library Journals Frontfile Complete
subjects Cycles
Dendritic structure
Deposition
Electrolytes
Ion currents
Ionic liquids
Ions
Lithium
li‐metal batteries
localized highly concentrated electrolytes
nonflammable electrolytes
Photoelectrons
Raman spectroscopy
safe electrolytes
Separators
Solid electrolytes
Solvation
Solvents
Spectrum analysis
title Intrinsically Nonflammable Ionic Liquid‐Based Localized Highly Concentrated Electrolytes Enable High‐Performance Li‐Metal Batteries
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