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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 ,
Bo Hong,
Mengnan Wang,
Rui Tan ,
Serena Margadonna ,
Yanqing Lai,
Maria Magdalena Titirici
Advanced Science
Swansea University Authors: Zari Tehrani , Rui Tan , Serena Margadonna
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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...
Published in: | Advanced Science |
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ISSN: | 2198-3844 2198-3844 |
Published: |
Wiley
2024
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Online Access: |
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URI: | https://cronfa.swan.ac.uk/Record/cronfa68437 |
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 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. |
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Keywords: |
Battery safety, flame-retardant electrolytes, fluorinated phosphates, molecular design, solvation shell tuning |
College: |
Faculty of Science and Engineering |
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). 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. |