Fluoroether Design Enables High-Voltage All-Solid-State Lithium Metal Batteries.

Chen, Y; Yang, X; Wang, T; Tang, X; Li, D; Wang, S; Lei, Y; Han, Y; Chen, S; Armand, M; Aurbach, D; Wang, G

Fluoroether Design Enables High-Voltage All-Solid-State Lithium Metal Batteries.

Chen, Y Yang, X Wang, T Tang, X Li, D Wang, S

Lei, Y Han, Y Chen, S Armand, M Aurbach, D Wang, G

Permalink

Publisher:: WILEY-V C H VERLAG GMBH
Publication Type:: Journal Article
Citation:: Adv Mater, 2025, pp. e2506020
Issue Date:: 2025-07-01

Open Access

Copyright Clearance Process

Recently Added
In Progress
Open Access

This item is open access.

Adobe PDF

Download Published versionAdobe PDF (5.43 MB)

View on publisher's site

View statistics

Full metadata record

Field	Value	Language
dc.contributor.author	Chen, Y
dc.contributor.author	Yang, X
dc.contributor.author	Wang, T
dc.contributor.author	Tang, X
dc.contributor.author	Li, D
dc.contributor.author	Wang, S https://orcid.org/0009-0000-0519-4842
dc.contributor.author	Lei, Y
dc.contributor.author	Han, Y
dc.contributor.author	Chen, S
dc.contributor.author	Armand, M
dc.contributor.author	Aurbach, D
dc.contributor.author	Wang, G
dc.date.accessioned	2025-08-11T03:58:19Z
dc.date.available	2025-08-11T03:58:19Z
dc.date.issued	2025-07-01
dc.identifier.citation	Adv Mater, 2025, pp. e2506020
dc.identifier.issn	0935-9648
dc.identifier.issn	1521-4095
dc.identifier.uri	http://hdl.handle.net/10453/189351
dc.description.abstract	Developing high-voltage all-solid-state lithium metal batteries (ASSLMBs) holds transformative potential for next-generation energy storage technologies but remains a formidable challenge. Herein, a new prototype design is presented that integrates fluorinated ether segments into the traditional oxide nanocomposite phase, enabling poly(ethylene oxide)-based composite electrolytes with exceptional anti-oxidation durability and enhance overall electrochemical performance. Through a combination of experimental and computational analyses, it is demonstrated that the superior performance is attributed to the formation of reconstructed Li⁺ solvation with weakly coordinating environments. The proposed formulation exhibits excellent Li-metal compatibility, enabling stable cycling in symmetric Li\|\|Li cells for over 9500 h. The solid-state electrolyte also exhibits outstanding high-voltage stability with LiNi0.8Co0.1Mn0.1O2 cathodes, extending the operational voltage from 4.0 to 4.5 V. Moreover, the LiMn1-xFexPO4\|\|Li cells have delivered remarkable cycling performance, achieving over 1200 cycles with 99% capacity retention after 500 cycles. This work establishes an innovative platform for designing electrolytes with superior antioxidation properties and enhance structural durability, paving the way for the advancement of high-voltage all-solid-state lithium metal batteries.
dc.format	Print-Electronic
dc.language	eng
dc.publisher	WILEY-V C H VERLAG GMBH
dc.relation	http://purl.org/au-research/grants/arc/LP200200926
dc.relation.ispartof	Adv Mater
dc.relation.isbasedon	10.1002/adma.202506020
dc.rights	info:eu-repo/semantics/openAccess
dc.subject	02 Physical Sciences, 03 Chemical Sciences, 09 Engineering
dc.subject.classification	Nanoscience & Nanotechnology
dc.subject.classification	34 Chemical sciences
dc.subject.classification	40 Engineering
dc.subject.classification	51 Physical sciences
dc.title	Fluoroether Design Enables High-Voltage All-Solid-State Lithium Metal Batteries.
dc.type	Journal Article
utslib.location.activity	Germany
utslib.for	02 Physical Sciences
utslib.for	03 Chemical Sciences
utslib.for	09 Engineering
pubs.organisational-group	University of Technology Sydney
pubs.organisational-group	University of Technology Sydney/Faculty of Science
pubs.organisational-group	University of Technology Sydney/Faculty of Science/School of Mathematical and Physical Sciences
pubs.organisational-group	University of Technology Sydney/UTS Groups
pubs.organisational-group	University of Technology Sydney/UTS Groups/Centre for Clean Energy Technology (CCET)
utslib.copyright.status	open_access	*
dc.rights.license	This work is licensed under a Creative Commons Attribution 4.0 International License (CC BY 4.0). To view a copy of this license, visit https://creativecommons.org/licenses/by/4.0/
dc.date.updated	2025-08-11T03:58:15Z
pubs.publication-status	Published online

Abstract:

Developing high-voltage all-solid-state lithium metal batteries (ASSLMBs) holds transformative potential for next-generation energy storage technologies but remains a formidable challenge. Herein, a new prototype design is presented that integrates fluorinated ether segments into the traditional oxide nanocomposite phase, enabling poly(ethylene oxide)-based composite electrolytes with exceptional anti-oxidation durability and enhance overall electrochemical performance. Through a combination of experimental and computational analyses, it is demonstrated that the superior performance is attributed to the formation of reconstructed Li⁺ solvation with weakly coordinating environments. The proposed formulation exhibits excellent Li-metal compatibility, enabling stable cycling in symmetric Li||Li cells for over 9500 h. The solid-state electrolyte also exhibits outstanding high-voltage stability with LiNi0.8Co0.1Mn0.1O2 cathodes, extending the operational voltage from 4.0 to 4.5 V. Moreover, the LiMn1-xFexPO4||Li cells have delivered remarkable cycling performance, achieving over 1200 cycles with 99% capacity retention after 500 cycles. This work establishes an innovative platform for designing electrolytes with superior antioxidation properties and enhance structural durability, paving the way for the advancement of high-voltage all-solid-state lithium metal batteries.

Please use this identifier to cite or link to this item:

http://hdl.handle.net/10453/189351