Interfacial Chemistry-Driven Reaction Dynamics and Resultant Microstructural Evolution in All-Solid-State Batteries

Interfacial Chemistry-Driven Reaction Dynamics and Resultant Microstructural Evolution in All-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 Interfacial Chemistry-Driven Reaction Dynamics and Resultant Microstructural Evolution in All-Solid-State Batteries Sung-Kyun Jung, Chanhyun Park, Jingyu Choi, Seojoung Park, Hyeong-Jong Kim, and 11 more This is a preprint; it has not been peer reviewed by a journal. https://doi.org/ 10.21203/rs.3.rs-5739869/v1 This work is licensed under a CC BY 4.0 License Status: Published Journal Publication published 03 Oct, 2025 Read the published version in Nature Communications → Version 1 posted You are reading this latest preprint version Abstract Achieving a comprehensive understanding of battery systems necessitates multi-length scale analysis, spanning from the atomic to macro scale, to grasp the complex interplay of phenomena influencing performance. However, studies to understand these phenomena in all-solid-state batteries (ASSBs) poses significant challenges due to the complex microstructural evolution involved, such as the pore formation and contact loss resulting from cathode material breathing, chemical degradation at interfaces, and their interplay. Herein, we investigate the impact of chemical degradation at the cathode/solid-electrolyte interface on the cathode particle reaction behavior and microstructural evolution in composite cathodes of sulfide-based ASSBs, using a well-defined model system incorporating a non-decomposable coating layer that solely alters the interfacial chemical reactivity. By using lithium difluorophosphate (LiDFP) to suppress chemical degradation, we observed that this suppression enhances the reaction uniformity among particles and homogenizes mechanical degradation, albeit increasing pore formation and tortuosity. In addition, unbridled chemical degradation induces significant reaction heterogeneity and non-uniform mechanical degradation, with fewer pores and lower tortuosity. These findings complement the understanding of mechanical degradation, which is traditionally described using the metrics of contact loss and tortuosity, and underscore the critical role of coating layers in promoting lithium conduction by maintaining contact with the cathode surface. This research not only offers novel insights into the intertwined chemo-mechanical degradation and the functionality of the coating material but also paves the way for the multi-length scale understanding required for the development of advanced ASSBs. Physical sciences/Materials science/Materials for energy and catalysis/Batteries Physical sciences/Chemistry/Electrochemistry/Batteries All-solid-state Batteries Cathode–solid electrolyte interface Cathode reaction heterogeneity Digital twin 3D reconstruction Intertwined chemo-mechanical degradation Full Text Additional Declarations There is NO Competing Interest. Supplementary Files SupplementalVideo1.mp4 Supplemental video 1 SupplementalVideo2.mp4 Supplemental video 2 Supplementaryinformation.docx Supplementary information. Cite Share Download PDF Status: Published Journal Publication published 03 Oct, 2025 Read the published version in Nature Communications → 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. 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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-5739869","acceptedTermsAndConditions":true,"allowDirectSubmit":false,"archivedVersions":[],"articleType":"Article","associatedPublications":[],"authors":[{"id":401657214,"identity":"0f2b7d3d-63d5-4579-b2bf-2c32703542d2","order_by":0,"name":"Sung-Kyun 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