Difluoro-Modulated Molecular Interactions in Deep Eutectic Solid Polymer Electrolytes Enabling High-voltage Lithium-Metal Batteries

Difluoro-Modulated Molecular Interactions in Deep Eutectic Solid Polymer Electrolytes Enabling High-voltage Lithium-Metal Batteries | Authorea try { document.documentElement.classList.add('js'); } catch (e) { } var _gaq = _gaq || []; _gaq.push(['_setAccount', 'G-8VDV14Y67G']); _gaq.push(['_trackPageview']); (function() { var ga = document.createElement('script'); ga.type = 'text/javascript'; ga.async = true; ga.src = ('https:' == document.location.protocol ? 'https://ssl' : 'http://www') + '.google-analytics.com/ga.js'; var s = document.getElementsByTagName('script')[0]; s.parentNode.insertBefore(ga, s); })(); Skip to main content Preprints Collections Wiley Open Research IET Open Research Ecological Society of Japan All Collections About About Authorea FAQs Contact Us Quick Search anywhere Search for preprint articles, keywords, etc. Search Search ADVANCED SEARCH SCROLL Energy & Environmental Materials This is a preprint and has not been peer reviewed. Data may be preliminary. 13 May 2026 V1 Latest version Share on Difluoro-Modulated Molecular Interactions in Deep Eutectic Solid Polymer Electrolytes Enabling High-voltage Lithium-Metal Batteries Authors : Lehao Pan [email protected] , Yuying Zhang [email protected] , Haiyang Wang [email protected] , Liheng Zhang [email protected] , Tao You [email protected] , Xiaoye Jiang [email protected] , Longlong Wang [email protected] , Chen Wang 0009-0007-0167-097X [email protected] , and Lin Li [email protected] Authors Info & Affiliations https://doi.org/10.22541/authorea.15003289/v1 20 views 19 downloads Contents Abstract Supplementary Material Information & Authors Metrics & Citations View Options References Figures Tables Media Share Abstract Deep eutectic solid polymer electrolytes (DESPE) have emerged as promising candidates for high-safety, high-energy-density lithium-metal batteries. However, their practical application is hindered by unstable electrode–electrolyte interface. Herein, a difluoro-functionalized monomer, 2,2-difluoroethyl methacrylate (DFEMA), is rationally designed to regulate intermolecular interactions and solvation structure in DESPE. The moderated Li⁺ binding affinity in DFEMA-based systems facilitates Li⁺ desolvation and accelerates interfacial kinetics, resulting in enhanced ionic conductivity (0.79 mS cm⁻¹ at 30 °C) and a wide electrochemical stability window (up to 4.9 V vs. Li⁺/Li). Meanwhile, the tailored solvation environment promotes the formation of robust inorganic-rich interphases, including a stable solid electrolyte interphase (SEI) and cathode electrolyte interphase (CEI). Consequently, the resulting electrolyte enables ultralong cycling stability, sustaining over 1000 h in Li||Li symmetric cells and delivering 94.2% capacity retention after 450 cycles in 4.5 V LiCoO₂||Li full cells. This work highlights fluorination-degree regulation as an effective molecular design strategy for tailoring solvation chemistry and interfacial stability of solid polymer electrolytes for advanced high-voltage lithium metal batteries. Supplementary Material File (supporting information.docx) supporting information Download 26.60 MB Information & Authors Information Version history V1 Version 1 13 May 2026 Collection Energy & Environmental Materials Keywords energy materials in situ and operando characterization materials science batteries electrochemistry batteries electrolytes electrochemistry solar cells carbon materials nanotechnology photovoltaics materials science batteries electrolytes polymers surface and interface energy materials energy materials in situ and operando characterization materials science batteries electrochemistry energy materials semiconductors solar cells light emitting materials materials science batteries energy materials materials science batteries electrolytes electrochemistry solar cells carbon materials nanotechnology photovoltaics materials science Authors Affiliations Lehao Pan [email protected] Qingdao University, Qingdao, China View all articles by this author Yuying Zhang [email protected] Qingdao University, Qingdao, China View all articles by this author Haiyang Wang [email protected] Qingdao University, Qingdao, China View all articles by this author Liheng Zhang [email protected] Qingdao University, Qingdao, China View all articles by this author Tao You [email protected] Qingdao University, Qingdao, China View all articles by this author Xiaoye Jiang [email protected] Qingdao University, Qingdao, China View all articles by this author Longlong Wang [email protected] Qingdao University, Qingdao, China View all articles by this author Chen Wang 0009-0007-0167-097X [email protected] Qingdao University, Qingdao, China View all articles by this author Lin Li [email protected] Qingdao University, Qingdao, China View all articles by this author Metrics & Citations Metrics Article Usage 20 views 19 downloads .FvxKWukQNSOunydq8rnd { width: 100px; } Citations Download citation Lehao Pan, Yuying Zhang, Haiyang Wang, et al. Difluoro-Modulated Molecular Interactions in Deep Eutectic Solid Polymer Electrolytes Enabling High-voltage Lithium-Metal Batteries. Authorea . 13 May 2026. DOI: https://doi.org/10.22541/authorea.15003289/v1 If you have the appropriate software installed, you can download article citation data to the citation manager of your choice. Simply select your manager software from the list below and click Download. For more information or tips please see 'Downloading to a citation manager' in the Help menu . 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