Exploring the Interaction Between Particle Cracking and Expansion in NMC811 Using an Electro-Chemo-Mechanical Model

Exploring the Interaction Between Particle Cracking and Expansion in NMC811 Using an Electro-Chemo-Mechanical Model | 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 Exploring the Interaction Between Particle Cracking and Expansion in NMC811 Using an Electro-Chemo-Mechanical Model Vinit Nagda, Henrik Ekström, Artem Kulachenko This is a preprint; it has not been peer reviewed by a journal. https://doi.org/ 10.21203/rs.3.rs-6620040/v1 This work is licensed under a CC BY 4.0 License Status: Under Review Version 1 posted You are reading this latest preprint version Abstract Ni-rich cathode materials, such as NMC811, enable high-performance lithium-ion batteries but their polycrystalline structure predisposes them to particle cracking. Previous experimental research identified particle cracking as a significant degradation mechanism in Ni-rich cathodes, yet the counterintuitive volume expansion of secondary particles upon delithiation remained unexplained. This study employs a 3D electro-chemo-mechanical model with phase field fracture to investigate particle cracking's impact on electrochemical performance and volumetric expansion. Our analysis reveals that intergranular fracture, initiated by anisotropic deformation at grain interfaces, significantly impacts battery performance. Comparison between 2D and 3D modelling approaches establishes that three-dimensional models are essential for accurately capturing crack propagation patterns and their electrochemical consequences. Particle cracking temporarily reduces overpotential by increasing the electrochemically active surface area but may eventually promote side reactions, increasing resistance and reducing capacity. Furthermore, cracking leads to unexpected volumetric expansion of secondary particles despite unit-cell contraction during delithiation. Finally, the study examines mechanisms potentially driving this expansion: dynamic fracture events, electrolyte capillary forces, CEI formation, and residual stresses, concluding that residual stress release, particularly from electrode manufacturing processes, is the primary contributor. These findings show the critical need for controlling anisotropic strains and residual stresses to mitigate particle cracking and improve electrode stability. Physical sciences/Energy science and technology/Energy storage/Batteries Physical sciences/Mathematics and computing/Computational science Physical sciences/Engineering/Mechanical engineering Physical sciences/Chemistry/Electrochemistry/Batteries NMC Polycrystalline Cathode Phase field damage Electrolyte infiltration Residual stresses CEI Formation Irreversible growth Full Text Additional Declarations There is NO Competing Interest. Supplementary Files SupportingInformation.docx Supplementary Information Cite Share Download PDF Status: Under Review 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. 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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-6620040","acceptedTermsAndConditions":true,"allowDirectSubmit":false,"archivedVersions":[],"articleType":"Article","associatedPublications":[],"authors":[{"id":457479186,"identity":"48d7da96-070f-4f5e-8959-80e1cf7d3899","order_by":0,"name":"Vinit 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