High-Performance All-Solid-State Lithium Metal Batteries Enabled by Ionic Covalent Organic Framework Composites

High-Performance All-Solid-State Lithium Metal Batteries Enabled by Ionic Covalent Organic Framework Composites | Research Square window.SnipcartSettings = { analytics: { enabled: false } }; (function() { var accessVector = localStorage.getItem('access_vector') || ''; window.dataLayer = window.dataLayer || []; if (accessVector) { window.dataLayer.push({ user: { profile: { profileInfo: { snid: accessVector } } } }); } })(); (function(w,d,s,l,i){w[l]=w[l]||[];w[l].push({'gtm.start':new Date().getTime(),event:'gtm.js'});var f=d.getElementsByTagName(s)[0],j=d.createElement(s),dl=l!='dataLayer'?'&l='+l:'';j.async=true;j.src='https://www.googletagmanager.com/gtm.js?id='+i+dl;f.parentNode.insertBefore(j,f);})(window,document,'script','dataLayer','GTM-K279D39R'); Browse Preprints In Review Journals COVID-19 Preprints AJE Video Bytes Research Tools Research Promotion AJE Professional Editing AJE Rubriq About Preprint Platform In Review Editorial Policies Our Team Advisory Board Help Center Sign In Submit a Preprint Cite Share Download PDF Research Article High-Performance All-Solid-State Lithium Metal Batteries Enabled by Ionic Covalent Organic Framework Composites Jun Huang, Lei Cheng, Zhenyang Zhang, Chen Li, Ki-Taek Bang, Albert Liem, and 6 more This is a preprint; it has not been peer reviewed by a journal. https://doi.org/ 10.21203/rs.3.rs-4015490/v1 This work is licensed under a CC BY 4.0 License Status: Published Journal Publication published 27 Apr, 2024 Read the published version in Advanced Energy Materials → Version 1 posted You are reading this latest preprint version Abstract Ionic covalent organic frameworks (iCOFs) are crystalline materials with stable porous structures. They hold great potential for ion transport, particularly as solid-state electrolytes (SSEs) for all-solid-state Lithium metal batteries (ASSLMBs). However, achieving an ionic conductivity of over 10 −3 S cm −1 at room temperature using pure-iCOF-based SSEs, even adding additives such as lithium salts, is challenging as the voids work as strong resistances. Thus, highly conductive iCOFs typically require quasi-solid-state configurations with organic solvents or plasticizers. In this study, we prepared composites comprising iCOFs and poly(ionic liquid) (PIL) to make all-solid-state iCOFs electrolytes with an exceptional ionic conductivity up to 1.50 × 10 −3 S cm −1 and a high Li + transference number of > 0.80 at room temperature. Combined experimental and computational studies showed that the co-coordination and competitive coordination mechanism established between the PIL, lithium bis(trifluoromethanesulfonyl)imide (LiTFSI) and iCOFs enabled rapid Li + transport while restricting TFSI − movement. ASSLMB cells, made of composite SSEs and LiFePO 4 composite cathode, demonstrated an initial discharge capacity of 141.5 mAh g −1 at 1 C and r.t., with an impressive capacity retention of 87% up to 800 cycles. Overall, this work presents a breakthrough approach for developing advanced SSEs for next-generation high-energy-density ASSLMBs. Lithium metal batteries All-solid-state electrolytes Covalent organic frameworks Poly(ionic liquid) Full Text Additional Declarations The authors declare no competing interests. Supplementary Figures and Supplementary Tables are not available with this version. Cite Share Download PDF Status: Published Journal Publication published 27 Apr, 2024 Read the published version in Advanced Energy Materials → Version 1 posted You are reading this latest preprint version Research Square lets you share your work early, gain feedback from the community, and start making changes to your manuscript prior to peer review in a journal. As a division of Research Square Company, we’re committed to making research communication faster, fairer, and more useful. We do this by developing innovative software and high quality services for the global research community. Our growing team is made up of researchers and industry professionals working together to solve the most critical problems facing scientific publishing. Also discoverable on Platform About Our Team In Review Editorial Policies Advisory Board Help Center Resources Author Services Accessibility API Access RSS feed Manage Cookie Preferences © Research Square 2026 | ISSN 2693-5015 (online) Privacy Policy Terms of Service Do Not Sell My Personal Information {"props":{"pageProps":{"initialData":{"identity":"rs-4015490","acceptedTermsAndConditions":true,"allowDirectSubmit":true,"archivedVersions":[],"articleType":"Research Article","associatedPublications":[],"authors":[{"id":276420455,"identity":"aba42230-f3e8-47bb-a357-8b7175f34d5e","order_by":0,"name":"Jun Huang","email":"","orcid":"","institution":"","correspondingAuthor":false,"prefix":"","firstName":"Jun","middleName":"","lastName":"Huang","suffix":""},{"id":276420456,"identity":"e2b71a3f-4879-43f2-a0e5-f95b7c63c967","order_by":1,"name":"Lei 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4.0","url":"https://creativecommons.org/licenses/by/4.0/"},"manuscriptAbstract":"\u003cp\u003eIonic covalent organic frameworks (iCOFs) are crystalline materials with stable porous structures. They hold great potential for ion transport, particularly as solid-state electrolytes (SSEs) for all-solid-state Lithium metal batteries (ASSLMBs). However, achieving an ionic conductivity of over 10\u003csup\u003e−3\u003c/sup\u003e S cm\u003csup\u003e−1\u003c/sup\u003e at room temperature using pure-iCOF-based SSEs, even adding additives such as lithium salts, is challenging as the voids work as strong resistances. Thus, highly conductive iCOFs typically require quasi-solid-state configurations with organic solvents or plasticizers. In this study, we prepared composites comprising iCOFs and poly(ionic liquid) (PIL) to make all-solid-state iCOFs electrolytes with an exceptional ionic conductivity up to 1.50 × 10\u003csup\u003e−3\u003c/sup\u003e S cm\u003csup\u003e−1\u003c/sup\u003e and a high Li\u003csup\u003e+\u003c/sup\u003e transference number of \u0026gt; 0.80 at room temperature. Combined experimental and computational studies showed that the co-coordination and competitive coordination mechanism established between the PIL, lithium bis(trifluoromethanesulfonyl)imide (LiTFSI) and iCOFs enabled rapid Li\u003csup\u003e+\u003c/sup\u003e transport while restricting TFSI\u003csup\u003e−\u003c/sup\u003e movement. ASSLMB cells, made of composite SSEs and LiFePO\u003csub\u003e4\u003c/sub\u003e composite cathode, demonstrated an initial discharge capacity of 141.5 mAh g\u003csup\u003e−1\u003c/sup\u003e at 1 C and r.t., with an impressive capacity retention of 87% up to 800 cycles. Overall, this work presents a breakthrough approach for developing advanced SSEs for next-generation high-energy-density ASSLMBs.\u003c/p\u003e","manuscriptTitle":"High-Performance All-Solid-State Lithium Metal Batteries Enabled by Ionic Covalent Organic Framework Composites","msid":"","msnumber":"","nonDraftVersions":[{"code":1,"date":"2024-03-06 18:40:16","doi":"10.21203/rs.3.rs-4015490/v1","editorialEvents":[{"type":"communityComments","content":0}],"status":"published","journal":{"display":true,"email":"[email protected]","identity":"researchsquare","isNatureJournal":false,"hasQc":true,"allowDirectSubmit":true,"externalIdentity":"","sideBox":"","snPcode":"","submissionUrl":"/submission","title":"Research Square","twitterHandle":"researchsquare","acdcEnabled":true,"dfaEnabled":false,"editorialSystem":"","reportingPortfolio":"","inReviewEnabled":false,"inReviewRevisionsEnabled":true}}],"origin":"","ownerIdentity":"53071640-4c41-46a3-8b82-7ffc9185e6c8","owner":[],"postedDate":"March 6th, 2024","published":true,"recentEditorialEvents":[],"rejectedJournal":[],"revision":"","amendment":"","status":"published-in-journal","subjectAreas":[],"tags":[],"updatedAt":"2024-05-01T22:46:12+00:00","versionOfRecord":{"articleIdentity":"rs-4015490","link":"https://doi.org/10.1002/aenm.202400762","journal":{"identity":"advanced-energy-materials","isVorOnly":true,"title":"Advanced Energy Materials"},"publishedOn":"2024-04-27 22:46:12","publishedOnDateReadable":"April 27th, 2024"},"versionCreatedAt":"2024-03-06 18:40:16","video":"","vorDoi":"10.1002/aenm.202400762","vorDoiUrl":"https://doi.org/10.1002/aenm.202400762","workflowStages":[]},"version":"v1","identity":"rs-4015490","journalConfig":"researchsquare"},"__N_SSP":true},"page":"/article/[identity]/[[...version]]","query":{"redirect":"/article/rs-4015490","identity":"rs-4015490","version":["v1"]},"buildId":"qtupq5eGEP_6zYnWcrvyt","isFallback":false,"isExperimentalCompile":false,"dynamicIds":[84888],"gssp":true,"scriptLoader":[]}