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Constructing Quasi‐Localized High‐Concentration Solvation Structures to Stabilize Battery Interfaces in Nonflammable Phosphate‐Based Electrolyte

Chenyang Shi, Mengran Wang, Zari Tehrani Orcid Logo, Bo Hong, Mengnan Wang, Rui Tan Orcid Logo, Serena Margadonna Orcid Logo, Yanqing Lai, Maria Magdalena Titirici

Advanced Science, Volume: 12, Issue: 6, Start page: 2411826

Swansea University Authors: Zari Tehrani Orcid Logo, Rui Tan Orcid Logo, Serena Margadonna Orcid Logo

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DOI (Published version): 10.1002/advs.202411826

Abstract

Flame-retardant phosphate-based electrolytes effectively enhance lithium-ion battery safety but suffer from poor compatibility with graphite anodes and high-voltage cathodes, hindering scalability. Fluorinated phosphates, though widely used, increase interfacial resistance at the anode, degrading pe...

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Published in: Advanced Science
ISSN: 2198-3844 2198-3844
Published: Wiley 2025
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URI: https://cronfa.swan.ac.uk/Record/cronfa68437
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Fluorinated phosphates, though widely used, increase interfacial resistance at the anode, degrading performance. In this work, carbonate solvents with strong polarity are introduced to prevent tris(2,2,2-trifluoroethyl) phosphate (TFEP) from participating in the solvation structure of lithium ions. This strategy forms a quasi-localized high-concentration solvation structure, thereby restricting the reduction of TFEP and its impact on the graphite anode. The LiNi0.8Mn0.1Co0.1O2 (NCM811) | Graphite (Gr) pouch cell with optimized electrolyte exhibits a capacity retention rate of 80.1% after 370 cycles at 0.5C, which is much more stable than the electrolyte with TFEP-involved solvation structure (capacity retention rate: 47.1% after 300 cycles). The corresponding pouch cell with cut-off voltage to 4.5 V exhibits a capacity retention rate of 82.8% after 125 cycles, significantly outperforming cells employing commercial carbonate electrolytes (capacity retention rate: 56.9% after 125 cycles). Thus, the developed quasi-localized high-concentration solvation structure can effectively stabilize the electrode interface, greatly enhancing the cycling performance of phosphate-based flame-retardant electrolytes.</abstract><type>Journal Article</type><journal>Advanced Science</journal><volume>12</volume><journalNumber>6</journalNumber><paginationStart>2411826</paginationStart><paginationEnd/><publisher>Wiley</publisher><placeOfPublication/><isbnPrint/><isbnElectronic/><issnPrint>2198-3844</issnPrint><issnElectronic>2198-3844</issnElectronic><keywords>Battery safety, &#xFB02;ame-retardant electrolytes, &#xFB02;uorinated phosphates, molecular design, solvation shell tuning</keywords><publishedDay>10</publishedDay><publishedMonth>2</publishedMonth><publishedYear>2025</publishedYear><publishedDate>2025-02-10</publishedDate><doi>10.1002/advs.202411826</doi><url/><notes/><college>COLLEGE NANME</college><department>Engineering and Applied Sciences School</department><CollegeCode>COLLEGE CODE</CollegeCode><DepartmentCode>EAAS</DepartmentCode><institution>Swansea University</institution><apcterm>SU Library paid the OA fee (TA Institutional Deal)</apcterm><funders>The authors gratefully acknowledge the National Natural Science Foundation of China (No. 52034011 and 52101278), Central South University Research Programme of Advanced Interdisciplinary Studies (2023QYJC005), Young Elite Scientists Sponsorship Program by CAST (2023QNRC001), the Science and Technology Innovation Program of Hunan Province (2023RC3054), the Fundamental Research Funds for Central Universities of the Central South University (2022ZZTS0405). 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spelling 2025-02-25T10:55:02.3474337 v2 68437 2024-12-03 Constructing Quasi‐Localized High‐Concentration Solvation Structures to Stabilize Battery Interfaces in Nonflammable Phosphate‐Based Electrolyte fd8e614b01086804c80fbafa6fa6aaf5 0000-0002-5069-7921 Zari Tehrani Zari Tehrani true false 774c33a0a76a9152ca86a156b5ae26ff 0009-0001-9278-7327 Rui Tan Rui Tan true false e31904a10b1b1240b98ab52d9977dfbe 0000-0002-6996-6562 Serena Margadonna Serena Margadonna true false 2024-12-03 EAAS Flame-retardant phosphate-based electrolytes effectively enhance lithium-ion battery safety but suffer from poor compatibility with graphite anodes and high-voltage cathodes, hindering scalability. Fluorinated phosphates, though widely used, increase interfacial resistance at the anode, degrading performance. In this work, carbonate solvents with strong polarity are introduced to prevent tris(2,2,2-trifluoroethyl) phosphate (TFEP) from participating in the solvation structure of lithium ions. This strategy forms a quasi-localized high-concentration solvation structure, thereby restricting the reduction of TFEP and its impact on the graphite anode. The LiNi0.8Mn0.1Co0.1O2 (NCM811) | Graphite (Gr) pouch cell with optimized electrolyte exhibits a capacity retention rate of 80.1% after 370 cycles at 0.5C, which is much more stable than the electrolyte with TFEP-involved solvation structure (capacity retention rate: 47.1% after 300 cycles). The corresponding pouch cell with cut-off voltage to 4.5 V exhibits a capacity retention rate of 82.8% after 125 cycles, significantly outperforming cells employing commercial carbonate electrolytes (capacity retention rate: 56.9% after 125 cycles). Thus, the developed quasi-localized high-concentration solvation structure can effectively stabilize the electrode interface, greatly enhancing the cycling performance of phosphate-based flame-retardant electrolytes. Journal Article Advanced Science 12 6 2411826 Wiley 2198-3844 2198-3844 Battery safety, flame-retardant electrolytes, fluorinated phosphates, molecular design, solvation shell tuning 10 2 2025 2025-02-10 10.1002/advs.202411826 COLLEGE NANME Engineering and Applied Sciences School COLLEGE CODE EAAS Swansea University SU Library paid the OA fee (TA Institutional Deal) The authors gratefully acknowledge the National Natural Science Foundation of China (No. 52034011 and 52101278), Central South University Research Programme of Advanced Interdisciplinary Studies (2023QYJC005), Young Elite Scientists Sponsorship Program by CAST (2023QNRC001), the Science and Technology Innovation Program of Hunan Province (2023RC3054), the Fundamental Research Funds for Central Universities of the Central South University (2022ZZTS0405). R.T. acknowledges the RSC Researcher Collaboration Grant (C23-8220221815) and Royce Industrial Collaboration Grant (RICP-R4-100029). R.T. and Z.T. acknowledge the support from Royal Academy of Engineering. 2025-02-25T10:55:02.3474337 2024-12-03T09:42:11.5572894 Faculty of Science and Engineering School of Engineering and Applied Sciences - Chemical Engineering Chenyang Shi 1 Mengran Wang 2 Zari Tehrani 0000-0002-5069-7921 3 Bo Hong 4 Mengnan Wang 5 Rui Tan 0009-0001-9278-7327 6 Serena Margadonna 0000-0002-6996-6562 7 Yanqing Lai 8 Maria Magdalena Titirici 9 68437__33154__38e20232abf24d38875be39fb78fc4c8.pdf 68437.VOR.pdf 2024-12-17T11:06:15.2423260 Output 4473931 application/pdf Version of Record true © 2024 The Author(s). This is an open access article under the terms of the Creative Commons Attribution License (CC-BY 4.0). true eng https://creativecommons.org/licenses/by/4.0/
title Constructing Quasi‐Localized High‐Concentration Solvation Structures to Stabilize Battery Interfaces in Nonflammable Phosphate‐Based Electrolyte
spellingShingle Constructing Quasi‐Localized High‐Concentration Solvation Structures to Stabilize Battery Interfaces in Nonflammable Phosphate‐Based Electrolyte
Zari Tehrani
Rui Tan
Serena Margadonna
title_short Constructing Quasi‐Localized High‐Concentration Solvation Structures to Stabilize Battery Interfaces in Nonflammable Phosphate‐Based Electrolyte
title_full Constructing Quasi‐Localized High‐Concentration Solvation Structures to Stabilize Battery Interfaces in Nonflammable Phosphate‐Based Electrolyte
title_fullStr Constructing Quasi‐Localized High‐Concentration Solvation Structures to Stabilize Battery Interfaces in Nonflammable Phosphate‐Based Electrolyte
title_full_unstemmed Constructing Quasi‐Localized High‐Concentration Solvation Structures to Stabilize Battery Interfaces in Nonflammable Phosphate‐Based Electrolyte
title_sort Constructing Quasi‐Localized High‐Concentration Solvation Structures to Stabilize Battery Interfaces in Nonflammable Phosphate‐Based Electrolyte
author_id_str_mv fd8e614b01086804c80fbafa6fa6aaf5
774c33a0a76a9152ca86a156b5ae26ff
e31904a10b1b1240b98ab52d9977dfbe
author_id_fullname_str_mv fd8e614b01086804c80fbafa6fa6aaf5_***_Zari Tehrani
774c33a0a76a9152ca86a156b5ae26ff_***_Rui Tan
e31904a10b1b1240b98ab52d9977dfbe_***_Serena Margadonna
author Zari Tehrani
Rui Tan
Serena Margadonna
author2 Chenyang Shi
Mengran Wang
Zari Tehrani
Bo Hong
Mengnan Wang
Rui Tan
Serena Margadonna
Yanqing Lai
Maria Magdalena Titirici
format Journal article
container_title Advanced Science
container_volume 12
container_issue 6
container_start_page 2411826
publishDate 2025
institution Swansea University
issn 2198-3844
2198-3844
doi_str_mv 10.1002/advs.202411826
publisher Wiley
college_str Faculty of Science and Engineering
hierarchytype
hierarchy_top_id facultyofscienceandengineering
hierarchy_top_title Faculty of Science and Engineering
hierarchy_parent_id facultyofscienceandengineering
hierarchy_parent_title Faculty of Science and Engineering
department_str School of Engineering and Applied Sciences - Chemical Engineering{{{_:::_}}}Faculty of Science and Engineering{{{_:::_}}}School of Engineering and Applied Sciences - Chemical Engineering
document_store_str 1
active_str 0
description Flame-retardant phosphate-based electrolytes effectively enhance lithium-ion battery safety but suffer from poor compatibility with graphite anodes and high-voltage cathodes, hindering scalability. Fluorinated phosphates, though widely used, increase interfacial resistance at the anode, degrading performance. In this work, carbonate solvents with strong polarity are introduced to prevent tris(2,2,2-trifluoroethyl) phosphate (TFEP) from participating in the solvation structure of lithium ions. This strategy forms a quasi-localized high-concentration solvation structure, thereby restricting the reduction of TFEP and its impact on the graphite anode. The LiNi0.8Mn0.1Co0.1O2 (NCM811) | Graphite (Gr) pouch cell with optimized electrolyte exhibits a capacity retention rate of 80.1% after 370 cycles at 0.5C, which is much more stable than the electrolyte with TFEP-involved solvation structure (capacity retention rate: 47.1% after 300 cycles). The corresponding pouch cell with cut-off voltage to 4.5 V exhibits a capacity retention rate of 82.8% after 125 cycles, significantly outperforming cells employing commercial carbonate electrolytes (capacity retention rate: 56.9% after 125 cycles). Thus, the developed quasi-localized high-concentration solvation structure can effectively stabilize the electrode interface, greatly enhancing the cycling performance of phosphate-based flame-retardant electrolytes.
published_date 2025-02-10T08:12:33Z
_version_ 1829179965554294784
score 11.057796

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