[{"data":1,"prerenderedAt":-1},["ShallowReactive",2],{"doc-seo-333472-105":3,"detail-sidebar-cat-0-en-105":81,"doc-detail-333472-en":131},{"code":4,"msg":5,"data":6},0,"ok",{"site_id":7,"language":8,"slug":9,"title":10,"keywords":11,"description":12,"schema_data":13,"social_meta":74,"head_meta":76,"extra_data":78,"updated_unix":80},105,"en","introducing-a-catalytic-polymerization-approach-for-bottlebrush-vinylphosphonate-solid-polymer-electrolytes-with-ethylene-oxide-side-chains","Introducing a Catalytic Polymerization Approach for Bottlebrush Vinylphosphonate Solid Polymer Electrolytes with Ethylene Oxide Side Chains","","Synthesis of two vinylphosphonate-backbone monomers is carried out by installing different ethylene oxide side-chain lengths, followed by catalytic polymerization using a yttrium catalyst in a rare-earth-mediated group transfer route. The products (P1-VP with one ethylene oxide unit and P2-VP with two units) are characterized and processed with LiBF4 into solid polymer electrolyte films. Elongating the side chains lowers thermal degradation onset from 260 to 210 °C and further reduces it to 225 and 160 °C upon LiBF4 addition. The glass transition shifts from −48 to −67 °C, X-ray diffraction confirms complete amorphousness, and ionic conductivity reaches 1.8 × 10−5 and 8.2 × 10−5 S cm−1 at 60 °C, with Li-ion hopping activation energies of 0.57 and 0.47 eV, respectively. Oxidative stability extends up to 4.3 V versus Li+/Li, while high phosphonate content limits lithium transference numbers to 0.03 (P1-VP) and 0.12 (P2-VP) and yields critical current densities of 5 and 10 μA cm−2.",{"@graph":14,"@context":73},[15,34,56],{"@type":16,"itemListElement":17},"BreadcrumbList",[18,23,27,31],{"item":19,"name":20,"@type":21,"position":22},"https://docshare.wps.com","Home","ListItem",1,{"item":24,"name":25,"@type":21,"position":26},"https://docshare.wps.com/document/","Document",2,{"item":28,"name":29,"@type":21,"position":30},"https://docshare.wps.com/document/research-report/","Research & Report",3,{"item":32,"name":10,"@type":21,"position":33},"https://docshare.wps.com/document/introducing-a-catalytic-polymerization-approach-for-bottlebrush-vinylphosphonate-solid-polymer-electrolytes-with-ethylene-oxide-side-chains/333472/",4,{"url":32,"name":10,"@type":35,"image":36,"author":41,"headline":10,"publisher":44,"fileFormat":47,"inLanguage":8,"description":12,"dateModified":48,"datePublished":49,"encodingFormat":47,"isAccessibleForFree":50,"interactionStatistic":51},"DigitalDocument",{"url":37,"@type":38,"width":39,"height":40},"https://docshare.wps.com/thumbnails/introducing-a-catalytic-polymerization-approach-for-bottlebrush-vinylphosphonate-solid-polymer-electrolytes-with-ethylene-oxide-side-chains/333472.png","ImageObject",300,407,{"name":42,"@type":43},"Felix Montgomery","Person",{"url":19,"name":45,"@type":46},"DocShare","Organization","application/pdf","2026-10-28","2026-09-21",true,{"@type":52,"interactionType":53,"userInteractionCount":55},"InteractionCounter",{"@type":54},"ViewAction",11,{"@type":57,"mainEntity":58},"FAQPage",[59,65,69],{"name":60,"@type":61,"acceptedAnswer":62},"How are the vinylphosphonate monomers designed in this study?","Question",{"text":63,"@type":64},"Two monomers with a vinylphosphonate backbone are synthesized, each functionalized with different ethylene oxide side-chain lengths.","Answer",{"name":66,"@type":61,"acceptedAnswer":67},"What polymer electrolyte components are used to form the solid films?",{"text":68,"@type":64},"The polyvinylphosphonates are cast into solid polymer electrolyte films using LiBF4 as the conducting salt.",{"name":70,"@type":61,"acceptedAnswer":71},"How do side-chain length and LiBF4 affect thermal degradation and glass transition?",{"text":72,"@type":64},"Increasing side-chain length lowers thermal degradation onset from 260 to 210 °C, and LiBF4 reduces it further to 225 and 160 °C; 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Polym. Mater. 2025, 7, 2102−2111  \nRead Online  \n\n|  |  |  |  |  |  |\n| --- | --- | --- | --- | --- | --- |\n| ACCESS   | Metrics & More |  |  Article Recommendations |  | *sı Supporting Information |\n\nABSTRACT: In the first part of this study, we synthesized two monomers with a vinylphosphonate backbone, each functionalized with varying ethylene oxide side chains. These monomers were then catalytically polymerized using a yttrium catalyst in a rareearth metal-mediated group transfer polymerization. The resulting polyvinylphosphonates, containing either one ethylene oxide unit (P1-VP) or two units (P2-VP), were characterized and cast into solid polymer electrolyte films using LiBF4 as the conducting salt. The onset of thermal degradation decreases with the elongation of the side chains, from 260 to 210 °C, and further decreases with the addition of LiBF4 to 225 and 160 °C. The glass transition temperature of the polymers decreased with increasing side chain length from −48 to −67 °C while showing no melting transition. X-ray diffraction confirmed the fully amorphous character of these polymers. The ionic conductivity reached 1.8 × 10−5 and 8.2 × 10−5 S cm−1 for P1-VP and P2-VP at 60 °C, respectively, with activation energies for the Li-ion hopping of 0.57 and 0.47 eV. Moreover, the polymer electrolytes showed an oxidative stability of up to 4.3 V vs Li+/Li. However, the high ratio of phosphonate units in the polymers is hypothesized to be a bottleneck, limiting the lithium transference number to 0.03 for P1-VP and 0.12 for P2-VP and the critical current density to 5 and 10 μA cm−2.  \nKEYWORDS: solid polymer electrolyte, solid-state battery, lithium metal battery, ionic conductivity, polyvinylphosphonates  \n1. INTRODUCTION  \nWith the commercialization of lithium-ion batteries in the early 1990s, an era of significant advancements in energy storage technologies began. Their improvements in energy density,  \ncost efficiency, and portable consumer  \ncycling stability have greatly transformed electronics and electric vehicles (EVs).1,2  \nDespite these advancements, the energy density of LIBs is still limited by the capacity of graphite, which serves as the primary anode material with a capacity of around 370 mA h g−1 .3 The greatest gain in energy density could be achieved by the implementation of lithium metal (LiM) anodes due to it having a high theoretical specific capacity (3860 mA h g−1), being the lightest metal (M = 6.94 g mol−1, ρ = 0.53 g cm−3), and having the lowest electrochemical potential (−3.04 V vs SHE).4−6 However, LiM anodes pose significant challenges due to inhomogeneous plating and stripping during cycling, which lead to dendrite formation. These dendrites can penetrate the separator within an organic liquid electrolyte, causing short-circuiting, rapid energy release, and, in the worstcase scenario, ignition of the electrolyte.7 Therefore, safer electrolyte alternatives were investigated, leading to the development of all-solid-state batteries (ASSBs). Herein, the organic liquid electrolytes in LiBs are substituted by an inorganic solid (oxides,8,9 sulfides,7 and halides10) or a polymer  \n© 2025 The Authors. Published by American Chemical Society  \nelectrolyte, which offer more resistance to dendrite penetration while at the same time increasing the electrochemical stability window to allow for the application of LiM anodes and potentially high-voltage cathode active materials as well.11, 12 Among the options, polymer electrolytes show the most promise for large-scale industrial applications due to their low cost, ease of processing, and compatibility with existing manufacturing technolo","cbCaioxLh2xjM7nZ","https://ap.wps.com/l/cbCaioxLh2xjM7nZ","pdf",2683718,"English","# Abstract\n## Introduction","[{\"question\":\"How are the vinylphosphonate monomers designed in this study?\",\"answer\":\"Two monomers with a vinylphosphonate backbone are synthesized, each functionalized with different ethylene oxide side-chain lengths.\"},{\"question\":\"What polymer electrolyte components are used to form the solid films?\",\"answer\":\"The polyvinylphosphonates are cast into solid polymer electrolyte films using LiBF4 as the conducting salt.\"},{\"question\":\"How do side-chain length and LiBF4 affect thermal degradation and glass transition?\",\"answer\":\"Increasing side-chain length lowers thermal degradation onset from 260 to 210 °C, and LiBF4 reduces it further to 225 and 160 °C; the glass transition decreases from −48 to −67 °C with no melting transition.\"}]","Introducing a Catalytic Polymerization Approach for Bottlebrush Vinylphosphonate Solid Polymer Electrolytes with Ethylene Oxide Side Chains | PDF",1790002606,25]