Enhanced Solid Polymer Electrolytes for Lithium Metal Batteries: In-situ cured Poly(ethylene oxide) with Lithium Imide and Bis(oxalato)borate salts

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Abstract

To address safety and energy density demands beyond conventional lithium-ion batteries, this study investigates solid polymer electrolytes (SPEs) for solid-state batteries (SSBs) featuring lithium metal anodes. We synthesize SPEs via in-situ polymerization using a poly(ethylene oxide) (PEO) matrix with LiFSI, LiTFSI, or LiBOB salts (5 wt% and 10 wt%). This in-situ method reduces PEO crystallinity, enhancing Li-ion conductivity and interfacial compatibility with electrodes. Results show that SPEs with 10 wt% salt, particularly LiFSI, exhibit the highest ionic conductivity (3.1 × 10⁻⁴ S cm⁻¹ at 25 °C and 6.0 × 10⁻⁴ S cm⁻¹ at 60 °C) and demonstrate superior cycling stability. While LiTFSI and LiBOB electrolytes display comparable initial conductivities, they suffer from limited cycle life. Electrochemical impedance spectroscopy (EIS) indicates this capacity fading stems from the growth of resistive interfacial layers. This work highlights the advantages of in-situ polymerization for SPEs, although mechanical stability requires further optimization to mitigate interfacial failure. These findings suggest LiFSI-based SPEs synthesized in-situ hold significant promise for developing safer, high-energy-density SSBs.
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Enhanced Solid Polymer Electrolytes for Lithium Metal Batteries: In-situ cured Poly(ethylene oxide) with Lithium Imide and Bis(oxalato)borate salts | 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 Search Search ADVANCED SEARCH SCROLL This is a preprint and has not been peer reviewed. Data may be preliminary. 26 August 2025 V1 Latest version Share on Enhanced Solid Polymer Electrolytes for Lithium Metal Batteries: In-situ cured Poly(ethylene oxide) with Lithium Imide and Bis(oxalato)borate salts Authors : Kato Daems 0000-0002-4547-3069 [email protected] , Olli Sorsa , Taina Rauhala , Seyedabolfazl Mousavihashemi , Marja Vilkman , Joeri Van Mierlo , and Maitane Berecibar Authors Info & Affiliations https://doi.org/10.22541/au.175617363.34373992/v1 169 views 128 downloads Contents Abstract Supplementary Material Information & Authors Metrics & Citations View Options References Figures Tables Media Share Abstract To address safety and energy density demands beyond conventional lithium-ion batteries, this study investigates solid polymer electrolytes (SPEs) for solid-state batteries (SSBs) featuring lithium metal anodes. We synthesize SPEs via in-situ polymerization using a poly(ethylene oxide) (PEO) matrix with LiFSI, LiTFSI, or LiBOB salts (5 wt% and 10 wt%). This in-situ method reduces PEO crystallinity, enhancing Li-ion conductivity and interfacial compatibility with electrodes. Results show that SPEs with 10 wt% salt, particularly LiFSI, exhibit the highest ionic conductivity (3.1 × 10⁻⁴ S cm⁻¹ at 25 °C and 6.0 × 10⁻⁴ S cm⁻¹ at 60 °C) and demonstrate superior cycling stability. While LiTFSI and LiBOB electrolytes display comparable initial conductivities, they suffer from limited cycle life. Electrochemical impedance spectroscopy (EIS) indicates this capacity fading stems from the growth of resistive interfacial layers. This work highlights the advantages of in-situ polymerization for SPEs, although mechanical stability requires further optimization to mitigate interfacial failure. These findings suggest LiFSI-based SPEs synthesized in-situ hold significant promise for developing safer, high-energy-density SSBs. Supplementary Material File (kd-lisaltcomparison-insitu-eem.pdf) Download 391.73 KB Information & Authors Information Version history V1 Version 1 26 August 2025 Copyright This work is licensed under a Non Exclusive No Reuse License. Keywords libob lifsi litfsi lithium salt comparison peo-based solid polymer electrolytes Authors Affiliations Kato Daems 0000-0002-4547-3069 [email protected] Vrije Universiteit Brussel View all articles by this author Olli Sorsa VTT View all articles by this author Taina Rauhala VTT View all articles by this author Seyedabolfazl Mousavihashemi VTT View all articles by this author Marja Vilkman VTT View all articles by this author Joeri Van Mierlo Vrije Universiteit Brussel View all articles by this author Maitane Berecibar Vrije Universiteit Brussel View all articles by this author Metrics & Citations Metrics Article Usage 169 views 128 downloads .FvxKWukQNSOunydq8rnd { width: 100px; } Citations Download citation Kato Daems, Olli Sorsa, Taina Rauhala, et al. Enhanced Solid Polymer Electrolytes for Lithium Metal Batteries: In-situ cured Poly(ethylene oxide) with Lithium Imide and Bis(oxalato)borate salts. Authorea . 26 August 2025. DOI: https://doi.org/10.22541/au.175617363.34373992/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 . Format Please select one from the list RIS (ProCite, Reference Manager) EndNote BibTex Medlars RefWorks Direct import Tips for downloading citations document.getElementById('citMgrHelpLink').addEventListener('click', function() { popupHelp(this.href); return false; }); $(".js__slcInclude").on("change", function(e){ if ($(this).val() == 'refworks') $('#direct').prop("checked", false); $('#direct').prop("disabled", ($(this).val() == 'refworks')); }); View Options View options PDF View PDF Figures Tables Media Share Share Share article link Copy Link Copied! Copying failed. 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