Granular Creep and Its Role in Optimizing Solid Electrolyte Fabrication for Solid-State Batteries

Granular Creep and Its Role in Optimizing Solid Electrolyte Fabrication for Solid-State Batteries | 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 Article Granular Creep and Its Role in Optimizing Solid Electrolyte Fabrication for Solid-State Batteries Howard Tu, Joseph Vazquez Mercado, Fernando D. Cúñez, Alhamdu Bage, and 3 more This is a preprint; it has not been peer reviewed by a journal. https://doi.org/ 10.21203/rs.3.rs-6248382/v1 This work is licensed under a CC BY 4.0 License Status: Posted Version 1 posted You are reading this latest preprint version Abstract The densification of solid electrolyte (SE) materials is crucial for improving the performance and stability of solid-state batteries. In this study, the role of granular creep in SE densification is investigated using numerical simulations and experimental validation on Li6PS5Cl (LPSCl) seperators. Using discrete element method (DEM) simulations, we analyze the influence of strain rate and cohesion on force chain evolution, particle rearrangement, and porosity reduction. Our results indicate that slow strain rates promote granular creep, allowing for gradual particle reorientation and stress relaxation, leading to higher packing density and lower residual porosity. To validate these findings, we also performed experiments at different strain rates, where X-ray computed tomography (XCT) and scanning electron microscopy (SEM) confirm that slow strain rates produce a more homogeneous microstructure. Furthermore, critical current density (CCD) tests on symmetric cells reveal that samples processed at the slowest strain rate exhibit a CCD of 3 mA/cm 2 , three times higher than samples processed at faster strain rates, highlighting the direct correlation between granular creep, densification, and ionic transport enhancement. These findings underscore the importance of strain-rate-controlled processing in optimizing SE microstructure, mechanical and electrochemical performance, offering insights into the fabrication of high-density, high-performance separators for next-generation solid-state batteries. Physical sciences/Energy science and technology/Energy storage/Batteries Physical sciences/Engineering/Mechanical engineering Physical sciences/Materials science/Structural materials/Ceramics All solid-state batteries Solid electrolyte fabrication Granular creep Cohesive granular materials Full Text Additional Declarations There is NO Competing Interest. Supplementary Files SupportInformation.pdf Supplementary Information Cite Share Download PDF Status: Posted 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-6248382","acceptedTermsAndConditions":true,"allowDirectSubmit":true,"archivedVersions":[],"articleType":"Article","associatedPublications":[],"authors":[{"id":437502186,"identity":"5aec8928-b31d-4e46-b8ca-9c0651f2e4d9","order_by":0,"name":"Howard Tu","email":"data:image/png;base64,iVBORw0KGgoAAAANSUhEUgAAAZAAAAAyAQMAAABI0h/eAAAABlBMVEX///8AAABVwtN+AAAACXBIWXMAAA7EAAAOxAGVKw4bAAAAvElEQVRIiWNgGAWjYBACAzDJBsTsDQwHgBRjA7FaJBh4DjAcOECaFokEBgaitJiz9xh+rihjqDO4+fbh4Q8MNrIbDhDQYtlzxljyzDkGCYPb6QZAh6UZE9RicCN3g2RjG0hLGsgvhxOJ0bL5J1jLzWMgLf+J0rINYssNNpCWA0RoOXP+m2XDOQnJmWeADjtjkGw8k6CW423JNxvKbPj5jh9j/lBRYSfbR0gLFEjATCBO+SgYBaNgFIwCAgAADORIow0Vz+gAAAAASUVORK5CYII=","orcid":"https://orcid.org/0000-0002-2345-799X","institution":"Rochester Institute of Technology","correspondingAuthor":true,"prefix":"","firstName":"Howard","middleName":"","lastName":"Tu","suffix":""},{"id":437502187,"identity":"54a58c2d-c0c4-4ade-94e6-eb04312cfd2a","order_by":1,"name":"Joseph Vazquez Mercado","email":"","orcid":"","institution":"Rochester Institute of Technology","correspondingAuthor":false,"prefix":"","firstName":"Joseph","middleName":"Vazquez","lastName":"Mercado","suffix":""},{"id":437502188,"identity":"d2b9455e-6e83-497d-998a-318e4f357b29","order_by":2,"name":"Fernando D. Cúñez","email":"","orcid":"https://orcid.org/0000-0002-1325-4654","institution":"Rochester Institute of Technology","correspondingAuthor":false,"prefix":"","firstName":"Fernando","middleName":"D.","lastName":"Cúñez","suffix":""},{"id":437502189,"identity":"52cb081a-401e-4f37-a5ec-4d41a986a506","order_by":3,"name":"Alhamdu Bage","email":"","orcid":"","institution":"Rochester Institute of Technology","correspondingAuthor":false,"prefix":"","firstName":"Alhamdu","middleName":"","lastName":"Bage","suffix":""},{"id":437502190,"identity":"8c07f257-78f2-4347-b77b-cf797057185a","order_by":4,"name":"Fengyu Shen","email":"","orcid":"","institution":"Lawrence Berkeley National Laboratory","correspondingAuthor":false,"prefix":"","firstName":"Fengyu","middleName":"","lastName":"Shen","suffix":""},{"id":437502191,"identity":"5d03f582-86e2-4937-9ce7-2059f7790467","order_by":5,"name":"Dilworth Parkinson","email":"","orcid":"","institution":"Lawrence Berkeley National Laboratory","correspondingAuthor":false,"prefix":"","firstName":"Dilworth","middleName":"","lastName":"Parkinson","suffix":""},{"id":437502192,"identity":"6d92aec8-5ecd-4f51-a296-0fbd6773bad5","order_by":6,"name":"Michael Tucker","email":"","orcid":"https://orcid.org/0000-0002-8508-499X","institution":"Lawrence Berkeley National Laboratory","correspondingAuthor":false,"prefix":"","firstName":"Michael","middleName":"","lastName":"Tucker","suffix":""}],"badges":[],"createdAt":"2025-03-18 01:40:36","currentVersionCode":1,"declarations":"","doi":"10.21203/rs.3.rs-6248382/v1","doiUrl":"https://doi.org/10.21203/rs.3.rs-6248382/v1","draftVersion":[],"editorialEvents":[],"editorialNote":"","failedWorkflow":false,"files":[{"id":98624956,"identity":"a09123eb-b2c4-4977-abba-b5f57d125366","added_by":"auto","created_at":"2025-12-19 17:08:51","extension":"pdf","order_by":1,"title":"","display":"","copyAsset":false,"role":"manuscript-pdf","size":3378179,"visible":true,"origin":"","legend":"Article File","description":"","filename":"GranularCreepanditsroleinSEsRIT.pdf","url":"https://assets-eu.researchsquare.com/files/rs-6248382/v1_covered_cb3b1c4c-6fc5-4cd7-9305-d44a8077617f.pdf"},{"id":79815764,"identity":"95ee04b9-dd6e-4b57-bfc8-7487296ddeb8","added_by":"auto","created_at":"2025-04-03 07:42:19","extension":"pdf","order_by":1,"title":"","display":"","copyAsset":false,"role":"supplement","size":643566,"visible":true,"origin":"","legend":"Supplementary Information","description":"","filename":"SupportInformation.pdf","url":"https://assets-eu.researchsquare.com/files/rs-6248382/v1/3bab696a2d40452130426541.pdf"}],"financialInterests":"There is \u003cb\u003eNO\u003c/b\u003e Competing Interest.","formattedTitle":"Granular Creep and Its Role in Optimizing Solid Electrolyte Fabrication for Solid-State Batteries","fulltext":[],"fulltextSource":"","fullText":"","funders":[],"hasAdminPriorityOnWorkflow":false,"hasManuscriptDocX":false,"hasOptedInToPreprint":true,"hasPassedJournalQc":"","hasAnyPriority":true,"hideJournal":true,"highlight":"","institution":"","isAcceptedByJournal":false,"isAuthorSuppliedPdf":true,"isDeskRejected":"","isHiddenFromSearch":false,"isInQc":false,"isInWorkflow":false,"isPdf":true,"isPdfUpToDate":true,"isWithdrawnOrRetracted":false,"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},"keywords":"All solid-state batteries, Solid electrolyte fabrication, Granular creep, Cohesive granular materials","lastPublishedDoi":"10.21203/rs.3.rs-6248382/v1","lastPublishedDoiUrl":"https://doi.org/10.21203/rs.3.rs-6248382/v1","license":{"name":"CC BY 4.0","url":"https://creativecommons.org/licenses/by/4.0/"},"manuscriptAbstract":"\u003cp\u003eThe densification of solid electrolyte (SE) materials is crucial for improving the performance and stability of solid-state batteries. In this study, the role of granular creep in SE densification is investigated using numerical simulations and experimental validation on Li6PS5Cl (LPSCl) seperators. Using discrete element method (DEM) simulations, we analyze the influence of strain rate and cohesion on force chain evolution, particle rearrangement, and porosity reduction. Our results indicate that slow strain rates promote granular creep, allowing for gradual particle reorientation and stress relaxation, leading to higher packing density and lower residual porosity. To validate these findings, we also performed experiments at different strain rates, where X-ray computed tomography (XCT) and scanning electron microscopy (SEM) confirm that slow strain rates produce a more homogeneous microstructure. Furthermore, critical current density (CCD) tests on symmetric cells reveal that samples processed at the slowest strain rate exhibit a CCD of 3 mA/cm\u003csup\u003e2\u003c/sup\u003e, three times higher than samples processed at faster strain rates, highlighting the direct correlation between granular creep, densification, and ionic transport enhancement. These findings underscore the importance of strain-rate-controlled processing in optimizing SE microstructure, mechanical and electrochemical performance, offering insights into the fabrication of high-density, high-performance separators for next-generation solid-state batteries.\u003c/p\u003e","manuscriptTitle":"Granular Creep and Its Role in Optimizing Solid Electrolyte Fabrication for Solid-State Batteries","msid":"","msnumber":"","nonDraftVersions":[{"code":1,"date":"2025-04-03 07:42:14","doi":"10.21203/rs.3.rs-6248382/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":"c3db9119-2a7b-4f83-a4a0-78e9fa28fb25","owner":[],"postedDate":"April 3rd, 2025","published":true,"recentEditorialEvents":[],"rejectedJournal":[],"revision":"","amendment":"","status":"posted","subjectAreas":[{"id":46585882,"name":"Physical sciences/Energy science and technology/Energy storage/Batteries"},{"id":46585883,"name":"Physical sciences/Engineering/Mechanical engineering"},{"id":46585884,"name":"Physical sciences/Materials science/Structural materials/Ceramics"}],"tags":[],"updatedAt":"2025-12-18T09:50:29+00:00","versionOfRecord":[],"versionCreatedAt":"2025-04-03 07:42:14","video":"","vorDoi":"","vorDoiUrl":"","workflowStages":[]},"version":"v1","identity":"rs-6248382","journalConfig":"researchsquare"},"__N_SSP":true},"page":"/article/[identity]/[[...version]]","query":{"redirect":"/article/rs-6248382","identity":"rs-6248382","version":["v1"]},"buildId":"8U1c8b4HqxoKbykW_rLl7","isFallback":false,"isExperimentalCompile":false,"dynamicIds":[84888],"gssp":true,"scriptLoader":[]}